Sandya S. A.
Athukoralalage
and
Nasim
Amiralian
*
Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, 4072, St Lucia, Queensland, Australia. E-mail: n.amiralian@uq.edu.au
First published on 18th August 2025
Surface-mediated pathogen transmission remains a critical vector for infectious disease, especially amidst biofilm-associated infections and rising antimicrobial resistance. This review critically examines the emergence of dual-functional surface coatings that integrate antimicrobial and antibiofouling strategies to provide continuous protection against microbial contamination. This paper investigates how recent innovations leverage physicochemical repulsion, contact-active biocides, controlled-release systems, and stimuli-responsive architectures to tackle both microbial adhesion and survival. This review spans applications across implants, wound dressings, filtration membranes, public touch surfaces, and marine systems, with a comparative lens on efficacy, biocompatibility, and long-term durability. Special attention is given to smart coatings that respond to stimuli (ex: pH, enzymes, and radiation) and nanocellulose-based systems as sustainable, tunable platforms. Despite significant advancements, challenges persist in balancing antimicrobial efficiency, surface stability, and ecological safety. We conclude by identifying key design principles and translational pathways for the development of next-generation multifunctional coatings capable of addressing complex microbial threats across healthcare, public and environmental interfaces.
Wider impactThe persistent threat of microbial contamination amplified by biofouling and antimicrobial resistance demands material solutions that move beyond conventional surface disinfection and single-function antimicrobial or antibiofouling coatings. This review presents a comprehensive overview of recently developed dual-functional surface coatings that integrate both these functionalities within a single interface. Key developments include the evolution of materials capable of preventing microbial adhesion while simultaneously inactivating pathogens through contact-active agents, controlled release systems, and stimuli-responsive architectures. A distinctive feature of this field is its cross-sector relevance: from medical implants and wound dressings to marine equipment and food-contact surfaces, and these coatings effectively address contamination risks in highly diverse environments. By critically analysing existing design strategies, translational barriers, and emerging platforms such as the application of dual-functional nanocellulose, this review offers a roadmap for scalable, durable, and biocompatible surface coating materials. As the field advances, insights from this review will guide the development of next-generation dual-functional coatings that are not only more effective but also more adaptable to real-world application demands. |
To address these intrinsic limitations, recent advancements have led to the development of dual-functional antimicrobial and antibiofouling coatings. As stated by Zou et al., “It takes walls and knights to defend a castle”,7 underscoring the concept of combining antibiofouling techniques with antimicrobial moieties. The integration of dual functions responds to the inherent limitations of single-mode strategies. Antibiofouling surfaces, such as superhydrophobic coatings and those modified with amphiphilic polymers like zwitterionic materials, can effectively repel bacterial attachment; however, they may not be able to eradicate microbes if adhesion does occur.8,9 Conversely, coatings that solely rely on antimicrobial agents (for example, those incorporating metal nanoparticles or antibiotics) offer high bactericidal activity but may suffer from issues such as cytotoxicity or the gradual development of bacterial resistance, or debris accumulation often impairs their long-term effectiveness.10–12
Although dual-functional coatings are increasingly recognised as a promising strategy for controlling pathogen transmission, most research to date remains narrowly focused on single-function coatings, primarily antibacterial materials. To highlight emerging interest in integrated approaches, we conducted a bibliometric analysis using Scopus. The search revealed that while publications on antimicrobial coatings have risen steadily from 2020 to 2025 due to the COVID-19 pandemic, studies explicitly reporting synergistic antimicrobial and antibiofouling functionalities remain comparatively limited (Fig. 1). This underscores a research gap and the need for more holistic surface engineering strategies that simultaneously prevent bacterial adhesion and eliminate pathogens. This review critically evaluates the current landscape of dual-functional surface coatings, with a focus on antibacterial applications across a range of settings, including healthcare, food-related applications, touch surfaces, and marine environments. Finally, we highlight the emerging role of nanostructured cellulosic materials as a sustainable and versatile platform for next-generation dual-functional coatings.
![]() | ||
| Fig. 2 Bacterial defences operate at multiple scales: (a) molecular–neutralisation and repair (b) cellular barriers, pumps, and motility and (c) multicellular biofilms, collective actions, and suicide, stress responses. Reproduced with permission from ref. 13 Copyright© 2023, Springer Nature Limited. | ||
Once bacteria encounter a surface, their adhesion is governed by weak physicochemical interactions, including hydrogen bonding, electrostatic forces, and van der Waals forces.14 The strength of bacterial adhesion and persistence on surfaces is determined not only by microbial surface structures but also by substrate properties, including surface roughness, porosity, charge distribution, and wettability,15,16 as well as environmental factors such as moisture, humidity and temperature. For a comprehensive overview of bacterial surface sensing and the physicochemical and biological factors influencing initial adhesion, readers are advised to refer to Zheng et al.16
Surface roughness plays a crucial role in bacterial adhesion, as increased roughness provides a larger surface area and structural support for bacterial attachment, protecting cells from shear forces. Consequently, bacterial adhesion and biofilm formation generally increase with surface roughness.16 However, porous surfaces, such as nanocellulose coatings, significantly reduce bacterial survival by inducing dehydration through droplet imbibition within the porous fibre network, creating an inhospitable environment.17 Surface charge also influences bacterial adhesion. Most bacteria possess a net negative charge due to carboxyl, amino, and phosphate groups on their cell walls, leading to stronger adhesion on positively charged surfaces.16 Hydrophobicity further affects bacterial colonisation, as hydrophobic surfaces reduce repulsive forces between the bacterial cell surface and the substrate, often promoting adhesion.18 In addition to surface properties, environmental conditions such as low ventilation and high humidity also contribute to bacterial persistence, as they create favourable conditions for nutrient availability.19
Following attachment, bacteria can transition into biofilms, embedding themselves within a self-produced extracellular matrix. The International Union of Pure and Applied Chemistry formally defines biofilms as: “An aggregate of microorganisms in which cells that are frequently embedded within a self-produced matrix of extracellular polymeric substance adhere to each other and/or to a surface”.20 National Institutes of Health estimates that over 80% of bacterial infections are accompanied by biofilm formation, and about 17 million new biofilm-associated infections annually arise in the United States.21
Biofilms are highly adaptable and respond dynamically to environmental conditions, including substrate hydration levels and metal ion availability. The influence of surface properties on biofilm formation is evident in E. coli AR3110, which adjusts its structure based on the water content of its substrate. On wet substrates, biofilms incorporate more water and dry mass, allowing them to spread over a larger area but making them mechanically softer. In contrast, biofilms on drier surfaces remain more compact, forming a denser and structurally rigid extracellular matrix.22 Biofilms of certain E. coli strains exhibit distinct mechanical responses to metal cations depending on their extracellular matrix composition. For example, biofilms co-producing curli and phosphoethanolamine (pEtN)-cellulose uniquely stiffen in the presence of trivalent cations such as Al(III) and Fe(III) but remain unaffected by bivalent cations like Zn(II) and Ca(II). In contrast, biofilms containing either curli or pEtN-cellulose alone do not show stiffness changes irrespective of cation valency, highlighting the complex interactions between biofilm composition and environmental factors.23 These adaptive responses not only influence biofilm structure but also contribute to bacterial survival advantages. Biofilms enhance microbial resilience by shielding bacteria from antimicrobial agents, facilitating nutrient exchange, and promoting horizontal gene transfer, which accelerates resistance development.13
| Antimicrobial material | Antimicrobial mechanism | Application |
|---|---|---|
| Quaternary ammonium (QA) | Cationic QA interacts with anionic phospholipids in bacterial membranes | Implant,24,25 contact surfaces,45 filtration membranes,46 biomedical,47 marine48,49 |
| 1-Bromo-dodecane | Positive charges disrupt bacterial membranes | Implant50 |
| Polyimidazolium (PIM) | Positive charges disrupt bacterial membranes | Wound dressing51 |
| Imidazolium-based zwitterionic polymers | Positively charged C2 carbon disrupts bacterial membranes | Contact surfaces52 |
| N,N-Dimethylaminoethyl methacrylate (DMAEMA) | Positive charges on the surface of protonated DMAEMA | Biomedical53 |
| Poly(dimethyl amino methyl styrene) (PDMAMS) | Positive charges disrupt bacterial membranes | Biomedical54 |
| Poly(hexamethylene biguanide) (PHMB) | Positive charges disrupt bacterial membranes | Implant55 |
| Antimicrobial peptides (AMP) | 1. Positive charges disrupt bacterial membranes 2. Penetrate the membranes through hydrophobic interactions | Implant,56–58 biomedical59 |
| Polylysine (PLYS) | Disrupt bacterial membranes through electrostatic interactions | Marine and biomedical60 |
| Triclosan | Inhibiting fatty acid synthesis in bacteria, which is crucial for building cell membranes and for reproducing | Implant50 |
| Poly(trimethylamino)ethyl methacrylate chloride (polyMETAC) | Electrostatic interactions between positively charged QA groups and negatively charged bacterial membranes | Implant61 |
| Iodine | Disrupts bacterial cell walls, oxidative damage and enzyme inhibition | Implants62 |
| Gentamicin | Binds to the bacterial ribosome, inhibiting protein synthesis, and causing cell death | Implant63,64 |
| Silver nanoparticles | Membrane disruption by positively charged Ag+ ions and ROS-mediated oxidative stress | Implant,65–67 contact surfaces,68 biomedical,69 textiles70 |
| Cu ions | ROS-mediated oxidative stress | Biomedical71 |
| N-Halamine structures | Release reactive chlorine species such as hypochlorous acid and hypochlorite ions → cell membrane damage, oxidize proteins, nucleic acids, and enzymes. | Food containers36 |
| Carboxymethyl chitosan–zinc oxide (CMC–ZnO) | UV-induced ROS from ZnO. Electrostatic interactions with chitosan's protonated –NH3+ | Marine37 |
| g-C3N4 nanosheets | Photocatalytic activity | Marine72 |
| Nitric oxide (NO) releasing compounds | NO disrupts bacterial cell membranes & inhibits respiration & DNA synthesis. | Implant,58,73 marine74 |
| Curcumin | Membrane disruption | Implant75 |
| EndLys enzyme | Hydrolyses the peptidoglycan layer of bacteria | Wound dressing76 |
| Houttuynia and scutellarin extracts | Contain bioactive compounds like decanal and safrole, which can disrupt bacterial cell walls and membranes. | Marine and biomedical77 |
| Au nanoparticles | Raising the surface temperature under 808 nm NIR irradiation | Implant78 |
Release-based coatings include agents such as phenolics, alcohols, aldehydes, halogens, oxidising agents, heavy metals, essential oils, and quaternary ammonium compounds (QACs) that gradually diffuse from the coating.24–26 Metal nanoparticles have received particular attention due to their efficacy in killing pathogens.27 Among different metal nanomaterials, silver,28 copper,29 and iron oxides such as Fe2O3 and Fe3O430 have attracted significant attention due to their proven contact-active antimicrobial properties.31,32 The major drawback with antimicrobial agents is their finite lifespan, as antimicrobial agents deplete, the surface loses its effectiveness.33 Additionally, the uncontrolled release of antimicrobial agents raises concerns regarding environmental toxicity34 and the potential for antimicrobial resistance.35
Contact-active coatings include cationic polymers or peptides that interact with bacterial membranes, N-halamines that transfer biocidal chlorine to bacterial cells,36 photocatalytic surfaces and nanoparticles that generate reactive oxygen species (ROS)37 and nanopillars penetrating membranes.38 While these coatings offer long-term antimicrobial activity without the depletion of active agents, efficacy may decrease over time due to surface degradation or biofouling, which can physically block active sites and promote bacterial colonisation.39 Additionally, prolonged exposure to these surfaces may lead to adaptive responses in bacteria such as membrane remodelling or efflux pump upregulation that could potentially contribute to the development of antimicrobial resistance.40,41
Stimuli-responsive antimicrobial coatings have been explored to overcome limitations, such as uncontrolled release and resistance development. Recent examples include poly(N-isopropylacrylamide-co-acrylic acid) microgel/polycaprolactone nanofibers that exhibit temperature-, pH-, and electro-responsive drug release, providing switchable antimicrobial action under specific triggers such as bacterial contamination (temperature, pH, electrical stimuli).42 Similarly, metal–organic framework (MOF)-based polypropylene coatings respond to bacterial metabolites by locally generating antibacterial nitric oxide (NO) radicals upon infection, offering precise microbial inactivation.43 Another innovative system involves thermo- and pH-responsive ciprofloxacin-loaded nanofibers that selectively release antibiotics under conditions typical of microbial colonisation, effectively reducing bacterial adhesion and biofilm formation.44
![]() | ||
| Fig. 3 (a) Schematic illustration of antibiofouling strategies and (b) key design strategies to impart antibiofouling properties to surface coatings. Reproduced with permission from ref. 79. Copyright 2020, John Wiley and Sons. | ||
Fouling-resistant surfaces repel the adhesion of pathogens through superhydrophobicity or hydration layers. Most efficient superhydrophobic coatings are combinations of nano/micro textures that have a rough patterned surface with empty concave domains and a layer of nonpolar compounds. Their durability is not affected by drug or ion release, and they repel both Gram (−) and Gram (+) bacteria. However, these coatings are challenging to produce at large scales, are expensive, and the patterns deform in contact with mechanical forces, thus, a defect in a coating will lead to bacterial attachment and consequent biofilm formation.80 On the other hand, hydrophilic antibiofoulants repel bacteria from the surface through the production of a strong hydration layer. They are mainly produced by grafting hydrophilic polymer chains containing oxygen-rich functionality onto the surface, which form hydrogen bonds with water and create a steric hindrance. In addition to directly resisting bacterial adhesion, these coatings also prevent the adsorption of proteins and other biomolecules that would otherwise form a conditioning layer on the surface.81 Since this layer promotes subsequent microbial colonisation, its absence makes the surface less hospitable to biofilm formation.
One of the most commonly used methods to impart antibiofouling properties to a surface is the application of polyethylene glycol (PEG)-based coatings through techniques such as physical or chemical adsorption, direct covalent attachment, and block or graft copolymerisation.82–85 However, PEG is susceptible to oxidative degradation, forming aldehydes and ethers, and loses its antibiofouling properties.79,86,87 Moreover, grafting PEG onto surfaces is a complex procedure and cannot easily scale up for economic surface coating.88,89 Zwitterionic polymers with covalently attached cation and anion pendant groups have been used to increase surface interactions with water and create antibiofouling properties.79 However, these polymers show the same drawback as PEG and are not stable at different temperatures and pH, limiting their application.90
Fouling-release surfaces are designed to permit only weak foulant adhesion, allowing foulants to be easily removed under low shear or mechanical force, such as water flow or manual cleaning. These coatings often utilise low-surface-energy materials like silicones and fluoropolymers, which reduce the interaction strength between the foulant and the substrate.79,91,92 In contrast, fouling-degrading surfaces contain active agents that target and degrade attached organic matter or kill adherent microorganisms. These may include oxidising agents or bactericidal functionalities embedded within the coating, which act upon contact with the fouling organism to chemically break down or eliminate it.79,93
Antibiofouling coatings cannot inactivate pathogens that may accumulate on compromised coating regions, eventually leading to biofouling.90 Once this occurs, foulants can mask antibiofouling functionalities, effectively turning an antibiofouling surface into a fouling-prone one. Without an antimicrobial mechanism, these coatings offer no defence beyond initial repulsion, making them vulnerable to delayed but persistent microbial colonisation. Moreover, under high bacterial loads, antibiofouling coatings can be overwhelmed, allowing bacterial outgrowth and eventual surface colonisation.94,95 This highlights a key limitation of antibiofouling-only approaches and sets the stage for dual-functional coatings, which combine passive repellence with active antimicrobial strategies (Table 2).
| Antibiofouling mechanism | Antibiofouling materials | Application |
|---|---|---|
| Steric repulsion created by the hydration layer | Poly(N-vinylpyrrolidone) (PVP) | Implant,25,62,75 biomedical54 |
| Hyaluronic acid (HA) | Implant24 | |
| N-(2-Hydroxypropyl)methacrylamide (pHPMA) | Wound dressing76 | |
| N,N-Dimethylaminoethyl methacrylate (DMAEMA) | Biomedical53 | |
| 2-Methacryloyloxyethyl phosphorylcholine, 3-methacryloxypropyl trimethoxysilane, and 3-(methacryloyloxy) (PMMMSi) | Biomedical59 | |
| Zwitterionic polymers | Implant,55,63,66,67 contact surfaces,45,52 biomedical,47,69,71 | |
| N-(3-Aminopropyl) methacrylamide (PDMA) | Implant56 | |
| Poly(ethylene glycol) (PEG) | Implant,57,64,78 Wound dressing,51 biomedical59 | |
| Heparin | Implant73 | |
| P(NIPAM-co-DMAPMA) | Implant50 | |
| PolyHEAA | Implants61 | |
| 2-Hydroxyethyl methacrylate (HEMA) | Implants96 | |
| Fluorinated polyurethane | Marine37 | |
| Nanosilica resin and TEGO® Addibit EK 50 | Contact surfaces68 | |
| Laser-induced periodic surface structured (LIPSS) Ti | Implant65 | |
| Poly-Schiff base resin | Marine72 | |
| β-Poly(2-methacryloyloxyethyl phosphorylcholine) (PMPC) | Marine60 | |
| Surface hydrophobicity | Biocide 4,5-dichloro-2-octyl-4-isothiazolin-3-one (DCOIT) | Marine and biomedical49 |
| L-Tryptophan/picolinic acid/4-nitrophenyl-isothiocyanate organogel | Textiles70 | |
| Strong cationic QA attracts bacteria and disrupts their membranes, while the hydration layer prevents them from reattaching. | GMTA | Filtration membranes46 |
| Provides low surface energy, making it difficult for fouling organisms to attach to the surface | Methylphenyl silicone resin (MSR) | Marine77 |
| Creates a slippery, lubricated surface that prevents microorganisms from adhering, biomimetic cilia, infused with FSoil, move under the influence of an external magnetic field, further preventing the attachment of microorganisms | Methyl fluoro-silicone oil (FSoil) | Marine74 |
| UV-Triggered depolymerization | Lithium phenyl-2,4,6-trimethylbenzoylphosphinate | Marine48 |
A widely adopted design principle involves combining antibiofouling polymers such as zwitterionic brushes101,102 or PEG derivatives103 with contact-active or stimuli-responsive bactericidal agents. The majority of current dual-functional coatings create robust hydration layers that prevent non-specific adhesion, while integrated biocides such as quaternary ammonium salts (QAS),101 cationic terpolymers,104 biguanide polymers,55 lysozyme,105 copper ions (Cu2+),71,106 silver nanoparticles (AgNPs),69 antimicrobial peptides (AMPs)59 and curcumin75,103 disrupt bacterial membranes or interfere with key metabolic processes. This dual-action mechanism enhances long-term performance: antibiofouling components minimise initial microbial adhesion, while antimicrobial agents inactivate/kill any organisms that overcome the passive barrier. A schematic illustration of this synergistic process is shown in Fig. 4. Dual-functional coatings can be further advanced by integrating stimuli-responsive properties, which dynamically alter the coating's physicochemical properties in response to specific environmental cues such as external triggers (ex, radiation) or bacterial metabolites (ex, enzymes, acidic pH).107,108
![]() | ||
| Fig. 4 Schematic illustration of a dual-functional surface coating. Antibiofouling components repel pathogen adhesion, while antimicrobial moieties inactivate pathogens that reach the surface. | ||
574 HAIs occurring in adults admitted to public hospitals annually, resulting in 7583 deaths.109 Conventional antimicrobial treatments face limitations due to cytotoxicity and the development of antimicrobial resistance (AMR), leading to reduced bactericidal effects and increased bacterial pathogenicity. By 2050, it is estimated that 10 million lives annually will be lost due to AMR, highlighting the urgent need for alternative strategies.110Table 3 provides a comparative overview of dual-functional coatings in healthcare, offering insight into the design–performance relationships critical for clinical translation.
| Dual-functional material | Contact angle (CA) | Zeta potential | Coating technique/surface texturing | Antimicrobial activity comes from | Antibiofouling activity comes from | Biocompatibility | Stability |
|---|---|---|---|---|---|---|---|
| Implants | |||||||
| Poly(N-vinylpyrrolidone-co-ethylene glycol dimethacrylate) (PVE)/iodine PVE–I62 | 67.0° | — | Initiated chemical vapour deposition (iCVD) | Iodine. | PVE | Good in vivo biocompatibility | Stable after 12 h at 37 °C; no FTIR changes, WCA shift from 55.4° to 56.2° |
| Killed 100% of E. coli and 91.80% of S. aureus. | |||||||
| Fe3O4@PDA–PEG nanoparticles in SF120 | — | — | — | Photothermal killing. Complete eradication of MRSA and E. coli | PEG-induced repulsion; SF limits bacterial contact | Excellent osteoblast viability | Maintains surface integrity after 8 weeks in PBS; no Fe3+ leaching detected |
| Polyurethane/Au/PEG78 | ∼60° | ∼−1.5 mV | Oxygen plasma treatment, thiol group introduction, and PEG post-modification | Au nanorods, 99.9% reduction under 808 nm NIR irradiation, raising the surface temperature to ∼55 °C. | PEG | Good cytocompatibility, hemolysis ratios <5% | Photothermal did not attenuate after 12 cycles of irradiation and cooling |
| Polydopamine/poly(GMA-co-DVBAPS) (PDA/L-PDV)124 | 18° (PEGDGE version) | — | Mussel-inspired PDA co-deposition on PP, PET, and catheters | Polylysine touch-killing | PEGDGE hydration; zwitterionic chain expansion | No toxicity reported | Maintained over 3 bacterial challenges with NaCl-triggered regeneration |
| QA/hydroxyethyl acrylate/PEG128 | ∼25° | — | In situ crosslinked polymer network on steel, Cu, Al | QA | Hydrophilic PEGA480 repels protein | Not cytotoxic; potential for surgical use | Self-healing at room temp; 93% mechanical recovery in 15 min |
| Polypropylene treated with polydopamine/QA/hyaluronic acid (PP-PDA-Q-HA)24 | 72° | +25.4 mV | PDA coating & chemical grafting | QA: Innactivations – 93% S. aureus, 93% E. coli, and 85% C. albicans. | HA: Inhibited 53% of S. aureus biofilm formation. | Good hemocompatibility, cytocompatibility & high cell viability | Retained antibacterial activity over 5 cycles |
| DMA-MPC-MPA-N+101 | ∼60° | — | Mussel-inspired dopamine terpolymer on PDMS | MPA-N+ quaternary ammonium (contact-kill) | MPC zwitterionic protein repellency | Hemolysis rate 1.73%; no cytotoxicity to smooth muscle cells | Stable in PBS at 37 °C over 21 days |
| Zwitterionic poly(sulfobetaine methacrylate-co-dopamine methacrylamide)/gentamicin sulphate (PSB/GS)63 | WCA of 35.3 ± 1.6° | — | Dopamine-assisted co-deposition of PSBDA and covalently linking GS | Zone of inhibition against E. coli and S. aureus due to GS | Zwitterionic PSBDA > 90% resistance to protein and bacterial adhesion | Hemolysis rate < 5%, no significant inflammatory response in vivo. good cytocompatibility | The cumulative release of GS reached 29 μg at pH 5.5 after 30 days |
| Laser-induced periodic surface structured Ti modified with polydopamine-chitosan–silver nanoparticles (Ti-PCA @LIPSS)65 | 20.2° ± 0.7° | — | Electroless plating | Silver ions, chitosan | LIPSS topography | Excellent biocompatibility and low toxicity to mammalian cells. | — |
| Curcumin/poly(N-vinylpyrrolidone)-co-poly(3-(acrylamido)phenylboronic acid) (PVP-co-PAPBA).75 | 34.17 ± 0.93° | — | Visible-light-induced graft polymerisation | Curcumin: Inactivation: 90.9% E. coli & 92.2% S. aureus. | PVP 93.4% reduction in platelet adhesion | Non-hemolytic properties, no cytotoxicity | Curcumin release was stable at pH 7.4 over 14 days, increased at pH 5.0, leading to an acidic responsiveness property |
| AgNPs/PMPD66 | 24.9 ± 3.1° | — | Dopamine-assisted coating | AgNPs 97% against E. coli and 99% against S. aureus. | Zwitterionic copolymer (P(DMA-co-MPC)) | Good hemocompatibility, highly biocompatible | WCA remained 28.0°–35.7° after 30 tape cycles: no WCA or thickness change after 12 h PBS flow |
| Cu2+-d-Met MOF106 | ∼50° | — | MPN chelation + Cu2+/d-Met MOF mineralization | Cu2+ catalytic ROS + d-Met biofilm dispersion | Chiral MOF disassembly + hydrophilicity | — | Retained Cu2+ release over 10 days: robust marine durability |
| ZIF-90-Bi-CeO2 hydrogel122 | Superhydrophilic | Hydrogel embedding + nanoparticle incorporation on Ti | Bi-mediated photothermal killing and Zn2+ release | CeO2 antioxidant modulation + hydration | Reduced inflammation; MSC-compatible | Effective across pH & in vivo; Zn2+ release under acidic conditions | |
| AMN/poly(B5AMA)/poly(MPC-st-B5AMA)/AgNPs67 | <15° | — | Layer-by-layer coating. | AgNPs- releasing Ag+ → 90% killing S. aureus and E. coli | Poly(B5AMA) and zwitterionic 2-MPC | Non-toxic and cell-adhesive. | |
| Well-defined biocompatibility even with AgNPs incorporation | 90% recovery in nano scratch test; complete macro-scratch healing within 1 min using 5 μL water | ||||||
| Poly(sulfobetaine methacrylate) (pSBMA)/N-hydroxysuccinimide methacrylate (NHSMA)/poly(hexamethylene biguanide) (PHMB)55 | 70° | — | Layer-by-layer construction | PHMB 100% antibacterial efficiency against E. coli and S. aureus | Zwitterionic pSBMA | No significant cytotoxicity | — |
| Si-PHB@Qe96 | ∼62° | — | Surface-grafted poly(HEMA-co-APBA) via SI-ATRP | pH-triggered Qe release (quorum sensing inhibition) | Hydration barrier from HEMA | L929 cell viability >90% | Maintained over 72 h; repeated Qe release cycles |
| Antimicrobial peptides/polydopamine/poly(N,N-dimethylacrylamide)/N-(3-aminopropyl) methacrylamide/iodoacetic acid. (AMPs/PDA/PDMA/APMA/IAA)56 | 37.9 ± 0.9° | — | Self-assembly | AMPs | PDMA: Reduced bacterial adhesion by 98.4% for S. saprophyticus and 97.5% for P. aeruginosa | Not hemolytic, high biocompatibility. | No change in thickness after being immersed in PBS for 7 days at 37 °C or after 10 min of ultrasonication |
| PEG and cationic polypeptide57 | 38.4° | — | Dopamine-assisted dip coating | Cationic polypeptide | PEG | Negligible hemolysis, no inflammatory response after 7 days of implantation. | Minimal thickness change after 24 h in water; retained integrity after 1 week in proteinase/lipase |
| Silicone rubber/S-nitroso-N-acetylpenicillamine/Nisin (SR-SNAP-Nisin)58 | 68.7 ± 4.7° | n/a | Dopamine-assisted dip coating | Nisin and NO-S. aureus: 99.55%, E. coli: 96.87% reduction | Nisin and NO -S. aureus: 99.91%, E. coli: 99.99% reduction | No cytotoxicity | Nisin on the PDA coatings is stable for over 120 hours |
| Heparin/S-nitroso-N-acetylpenicillamine – silicon rubber (Hep-NO-SR)73 | 65.3° ± 2.6 | n/a | Self-assembly | S-Nitroso-N-acetylpenicillamine (SNAP) → NO Release. A reduction of 99.46 ± 0.17% | Heparin # of viable adhered bacteria reduced by 92.6 ± 2.3% reduced platelet adhesion by 84.12 ± 6.19% | No signs of hemolytic activity, no significant cytotoxic response | Consistent NO flux over two weeks |
| Heparin reduced SNAP leaching pNO@TNT//pBA121 | — | — | Layer-by-layer NIR-sensitive NO donor grafting on TNT | NIR-triggered NO burst (MRSA, E. coli) | NO-induced disruption; indirect effect | Osteogenic promotion | Stable release modes under infection vs. physiological pH |
| Triclosan/quaternized P(NIPAM-co-DMAPMA)50 | — | +33.6 ± 1.1 mV | Spray coating on a polyanionic anchoring layer | 1-Bromo-dodecane | P(NIPAM-co-DMAPMA) | — | Stable after agitation and 48 h ethanol immersion with no observable changes |
| NVP/GMA-MPA-N+25 | 42.62 ± 4.12° | — | Surface grafting: RAFT | QA | NVP | Hemolysis ≤2%. | n/a |
| High cell viability | |||||||
| PolyHEAA/polyMETAC61 | ∼4° | 10 mV at neutral pH | Grafting onto a silica surface: SI-ATRP and SI-PIMP | PolyMETAC brush | PolyHEAA | Retain cell viability as high as 93%. | n/a |
| Gentamicin/poly(ethylene glycol) diglycidyl ether/ethylene glycol diglycidyl ether/ethylenediamine/polydopamine64 | 51.5° | — | Polydopamine (PDA) adhesive layer, followed by immersion in polymer solutions | Gentamicin | PEG | Non-toxic | No inhibition zone – coating remained stable and undissolved on the titanium disk |
| Wound dressing | |||||||
| PEG/PIM-Mal/NAC51 | — | — | Film: solution casting, fibres: syringe extrusion into CaCl2(aq) | PIM | Hydrogel network of PEG and PIM destroys biofilms | Low acute toxicity and good biocompatibility | Swelled 10–12 times in 60 min; tensile strength 4–5 kPa, strain 50–58% |
| pHPMA/EndLys76 | — | — | Self-assembly on an electrospun PCL mesh | EndLys | pHPMA | Biocompatible and non-toxic to human cells | Remained intact after 32 days in PBS and LB + FBS, and even after 180 days. |
| Not damaged by gamma irradiation | |||||||
| Other biomedical applications | |||||||
| Thymol/DMAEMA/BP53 | — | — | Photocuring | Positive charges on the surface of protonated DMAEMA. 100% against E. coli, S. aureus, and MRSA. | DMAEMA blocks inhibit 95% of S. aureus and 81% of E. coli biofilms. | Good biocompatibility | Coating maintained its antibacterial properties for at least 30 days |
| Metal-polyphenol networks with discrete metal–organic frameworks (MPN-DMOF) | WCA ∼50° | >+15 mV | Self-assembly | Petal-like geometry disrupts the physiological structure of bacteria, DNA damage and cell apoptosis by ROS. | D-Methionine ligands act as molecular scissors, facilitating biofilm detachment. | Did not induce cytotoxicity | Nanoindentation Tests: The hardness values were measured as 40.59 ± 16.03 MPa for MPN and 3.17 ± 0.83 MPa |
| MPNs: tannic acid (TA), polyethyleneimine (PEI), and Cu2+ ions106 | |||||||
| PDA/MPF/MTF47 | 21± 1.2° | — | Self-polymerisation of PD → covalent grafting of copolymers | QA: reduced the survival rate; S. aureus: to 6.8%. | Zwitterionic MPF copolymer | Cell viability >94.3% for normal human lung fibroblast cells | Slight activity loss after 7-day PBS aging; S. aureus survival ↑ to 20%, E. coli ↑ to 15.4% |
| E. coli: to 1.2%. | Lower protein adsorption of 3% | ||||||
| AMP KR12/PEG@PMMMSi59 | <120° due to the presence of AMPs | +25 mV | Dip coating of PMMMSi and grafting PEG and KR12 | KR12 | PMMMSi and PEG | — | — |
| MPC-AEMA/AgNPs@tannic acid69 | <5° | — | Dip coating | AgNPs | p(MPC-st-AEMA) | Noncytotoxic | — |
| PDMAMS/EGDA/PVP54 | 31° | 16 mV at pH 7.2 | iCVD | PDMAMS-99.9% killing rate against E. coli and B. subtilis | PVP | No toxicity | No noticeable change after being shaken in deionised water at 200 rpm for 24 h |
| CuII-PCBDA71 | 19.2° | — | Dip-coating | Cu II: E. coli: >99.9% P. aeruginosa >99.9%, S. aureus >99.9%, C. albicans >99.9% reduction after 2 hours | Zwitterionic PCBDA: Pristine CL, 22.5 μg cm−2, Cu II-PCBDA-coated CL: 1.5 μg cm−2 (24 hours) | 100% cell viability when in direct contact with human corneal epithelial cells for 48 hours | The coating is stable after immersion in PBS and shaking for 7 days |
One widely studied antibiofouling agent is PEG, whose hydrophilic chains can reduce protein and bacterial adhesion. When combined with antimicrobial agents like polypeptides57 and gentamicin dual-functional coatings have been achieved.64 Since PEG is susceptible to oxidative degradation,64 researchers have increasingly turned to zwitterionic polymers, such as sulphobetaine methacrylate (PSB)63 and dopamine methacrylamide (DMA)101 for their improved stability and hydration-mediated fouling resistance. PSB coatings can maintain efficacy for up to 30 days.63 However, passive antibiofouling alone is insufficient for devices at high risk of infection. To address this, antimicrobial agents are combined with antibiofouling backbones. Chen et al. (2022) applied a terpolymer of DMA, 2-methacryloyloxyethyl phosphorylcholine (MPC), and maleopimaric acid-derived QAS (MPA-N+) to polydimethylsiloxane (PDMS) substrates.101 Cationic MPA-N+ achieved 1.00-log, 1.09-log, and 0.94-log reductions against S. aureus, E. coli, and Pseudomonas aeruginosa (P. aeruginosa), respectively. Zwitterionic MPC reduced nonspecific adsorption of BSA, lysozyme, and fibrinogen by over 80% and showed substantial disruption of biofilm structure after 5 days. An in vivo infection model demonstrated a 4.66-log reduction in E. coli colonisation on implants and reduced inflammation. The coating also showed excellent blood compatibility and negligible cytotoxicity. Peng et al. designed a zwitterionic silicone rubber coating incorporating poly(hexamethylene biguanide) (PHMB), a broad-spectrum antimicrobial.55 By optimising the polymer blend ratio, they achieved near-total bacterial inhibition while maintaining surface fouling resistance. While promising, such systems face challenges in tuning the release kinetics to match clinical needs, overly rapid release can exhaust the active agent prematurely, while slow release may leave early-stage infections unchecked. Other recent coating strategies include ε-polylysine immobilised via bovine serum albumin supramolecular assembly,114 protein-based films crosslinked with polyurethane and chitosan,115 RAFT-polymerised N-vinylpyrrolidone and maleopimaric acid quaternary ammonium cation,25 and antibiotic-loaded polyacrylate.116
Controlled release of biocidal agents is another key area of interest for dual-functional coatings, as it enables sustained antimicrobial efficacy while reducing the frequency of reapplication. Among these agents, AgNPs are particularly prominent due to their broad-spectrum antimicrobial activity and oxidative stress mechanisms. However, their use has raised growing concern due to the risk of silver ion leaching, environmental accumulation,117 and the growing risk of silver-resistant microbial strains.118 Under prolonged silver nanoparticles exposure, bacteria exhibited reduced membrane permeability, upregulation of efflux pumps, and increased expression of stress response and metal resistance genes. These adaptations contributed to significantly higher minimum inhibitory concentrations, indicating the development of silver resistance.118 To address these challenges Liu and colleagues embedded AgNPs in a polydopamine–phosphorylcholine copolymer matrix, which provided sustained release and reduced platelet adhesion to 9.88% of uncoated surfaces while inhibiting 97% of E. coli and 99% of S. aureus.66 Notably, this system retained antimicrobial efficacy after 30 tape-peeling cycles and prolonged phosphate-buffered saline (PBS) immersion. Compared to conventional AgNP coatings, this approach reduced silver ion leaching, mitigating associated risks. Poly(N-vinylpyrrolidone)–iodine (PVE–I) coatings demonstrate how balancing hydrophilicity and cross-linking density controls iodine release profiles. PVE–I-2 coatings, which release 82.44% of iodine within 60 minutes, showed superior efficacy, with inhibition zones of 2.00 cm for E. coli and 2.07 cm for S. aureus.62
Increasing attention has also been paid to “smart” coatings that respond to IRI-related stimuli such as pH, heat, or enzymatic activity. These systems offer the promise of localised, on-demand antimicrobial release, potentially avoiding toxicity to surrounding tissue. Zhao et al. developed a photothermal coating incorporating gold nanorods, which, under near-infrared (NIR) irradiation, achieved >99% bacterial killing and a reduction of bacterial adhesion by 99.9%.78 NIR-responsive materials are effective for even deep tissue treatments compared to UV or visible light, which penetrates only a few millimetres into biological tissues.119 Quan et al. (2024) also developed a NIR-responsive coating by embedding magnetite nanoparticles coated with a layer of polydopamine (PDA) and further functionalised with polyethylene glycol (Fe3O4@PDA-PEG) into a silk fibroin (SF) matrix on titanium surfaces. Upon 808 nm NIR exposure, the coating reached photothermal temperatures of ∼55 °C, leading to complete eradication of E. coli and MRSA biofilms within 5 minutes, with no bacterial regrowth observed over 24 hours.120 While effective, the need for external light activation may limit its use in deep tissue implants. Acid-sensitive systems, such as those using poly(vinylpyrrolidone)–boronate networks to release curcumin under infection-mimicking conditions, represent a more autonomous solution.75 Both Hou et al. and Ding et al. introduced stimuli-responsive dual-functional coatings activated by the combination of acidic infection microenvironments and NIR irradiation.121,122 In Hou's system, a titanium-based surface was engineered by integrating titania nanotubes (TNT) with nitric oxide (NO) donors and coated with polyphenylboronic acid (pBA), forming the pNO@TNT//pBA structure (Fig. 5(a)).121 Under infection-mimicking acidic conditions, the outer pBA layer detaches, exposing the NO donor (cupferron), which undergoes rapid decomposition upon NIR stimulation to release NO locally (Fig. 5(b)). This results in potent antibacterial activity, achieving 97.84% killing of MRSA and 98.28% of E. coli within 12 hours. The coating also demonstrated significant biofilm eradication and reduced MRSA survival in a rat femoral implant model after seven days (Fig. 5(c)). Once infection resolves, low-dose NO release continues slowly under physiological conditions, promoting osteogenic signalling and supporting implant integration.
![]() | ||
| Fig. 5 Fabrication, mechanism, and in vivo antibacterial performance of the NO releasing dual-functional titanium coating (pNO@TNT//pBA). (a) Schematic of coating fabrication: NO donors and dopamine hydrochloride (DA·HCl) are co-deposited onto TNT to form pNO@TNT, followed by surface grafting of pBA. (b) Under infection-mimicking acidic conditions and NIR irradiation, the coating releases NO. (c) MRSA survival after 7 days of implantation. Reproduced with permission from ref. 121. Copyright 2025 John Wiley and Sons. (d) Schematic illustration of the fabrication of Ti-PCA@LIPSS, where PCA refers to PDA and chitosan (CS) with AgNPs. (e) Representative SEM images of E. coli biofilm formation for a 24-h incubation time. Scale bars are 10 μm. Reproduced with permission from ref. 65. Copyright 2024 John Wiley and Sons. | ||
Similarly, Ding et al. developed a hyaluronic acid/gelatine hydrogel coating embedded with zeolitic imidazolate framework-90-Bi-CeO2 nanoparticles.122 Upon 808 nm NIR exposure, the bismuth component produced localised heating, resulting in ∼95% biofilm eradication of S. aureus within 10 minutes. The coating also provided antioxidant protection via CeO2 and Zn2-mediated bioactivity, offering a synergistic platform for both infection control and healing. Zou et al. reported surface-grafted copolymer brushes of 2-hydroxyethyl methacrylate (HEMA) and 3-(acrylamide)phenylboronic acid, into which quercetin (Qe), a natural antibiofilm molecule, was immobilised via pH-sensitive boronate ester bonds.96 The poly(HEMA) layer reduces bacterial adhesion in the first 4 hours by >80%, without contact killing. Upon bacterial colonisation and subsequent acidification of the microenvironment, the boronate ester bonds cleave, releasing Qe to disrupt quorum sensing and inhibit biofilm maturation.
Additionally, enzyme-responsive coatings that harness bacterial protease activity, such as chitosan-hollow-nanosphere system loaded with eugenol and chrysophanol, offer a highly specific release mechanism, with efficacy sustained under physiological fluid flow for up to 30 days.123 Mao et al. (2021) engineered salt-responsive, substrate-independent implant coatings using PDA co-deposition with bactericidal polylysine, antibiofouling PEGDGE, and zwitterionic copolymer poly(GMA-co-DVBAPS).124 Coating achieved ∼93% killing of E. coli and ∼91% of S. aureus, as well as ∼94% bacterial release under 1 M NaCl, indicating salt-responsive detachment of adhered bacteria. Smart coatings featuring acid-triggered release of antimicrobial agents,75 thermoresponsive micellar assemblies immobilised on implantable surfaces,125 or antibiofilm peptides that modulate quorum-sensing pathways and suppress biofilm-associated gene expression56,126,127 represent a shift toward environmentally adaptive designs that deploy antimicrobial action only when needed, enhancing safety and longevity.
Another area of focus in dual-functional implant coatings is enhancing durability by integrating self-healing mechanisms,67,128 polymeric brush architectures,61 and antimicrobial functionalities.25 Aminomalononitrile (AMN)-based self-healing coatings maintained >90% bacterial inhibition against S. aureus and E. coli even after mechanical damage.67 Another example is hydroxyethyl acrylate (HEA), polyethylene glycol acrylate (PEGA480), and quaternised 4-vinylpyridine coating, which demonstrated >90% protein-repulsion efficiency and >99.9% bactericidal activity against S. aureus and E. coli after 1 hour.128 Upon surface damage, the supramolecular bonds enabled room-temperature self-healing, with mechanical recovery reaching 93% and complete antibacterial function restoration within 15 minutes. Polymer brush coatings incorporating cationic polyMETAC achieved a fivefold reduction in S. aureus adhesion and limited E. coli attachment to 1.8 × 105 cells per cm2, retaining low fouling levels even after 72 hours.61 Chemically modified antimicrobial surfaces, including quaternised polymers50 and rosin acid-based QAS,25 have demonstrated long-term antimicrobial effects, with a 99.99% bacterial killing efficacy against S. aureus and 86% reduction of bacterial adhesion and biofilm suppression for up to 21 days and a 4.89 log reduction in E. coli adhesion, respectively. Polysaccharide-based multilayer coatings achieved 93% inhibition of S. aureus and E. coli over five reapplication cycles while reducing hemolysis from 47% to 5%.24 Additionally, photocured coatings synthesised via ATRP reduced S. aureus biofilm formation by 95% and extended catheter lifespans from approximately 7 to 35 days in physiological environments.53 While these strategies collectively enhance coating stability and bacterial resistance, challenges remain in optimising antimicrobial potency while ensuring long-term mechanical resilience, biocompatibility, and resistance to biomolecular fouling, which are critical for clinical and industrial applications.
Surface engineering tactics, such as micropatterning on polypropylene,129 cicada wing-inspired topographies,130 or slippery liquid-infused porous surfaces infused with QAS,131 further amplify antibiofouling performance through physical disruption or lubricant-layer barriers. Most innovative recent developments incorporate both structural and chemical antimicrobial strategies. Laser-induced periodic surface structures (LIPSS) offer a physical mechanism to disrupt bacterial membranes via nanoscale topography, while chemical agents such as AgNPs contribute a sustained bactericidal effect.65 LIPSS-treated Ti substrates were further functionalised with a hybrid coating composed of PDA, chitosan, and AgNPs. PDA serves as a versatile adhesion promoter, enabling robust coating on the Ti surface and in situ reduction of Ag+ (Fig. 5(d)). Chitosan enhances both antimicrobial activity and biocompatibility. The resulting Ti-PCA@LIPSS combines mechano- and chemo-bactericidal functions, leading to significant reductions in E. coli biofilm formation over 24 hours (Fig. 5(e)), while also supporting fibroblast adhesion.
Dual-functional polyethylene glycol/polyimidazolium/N-acetylcysteine (PEG/PIM-Mal/NAC) hydrogel coating51 and N-(2-hydroxypropyl)methacrylamide/endolysin (pHPMA/EndLys) coated dressings76 offer distinct but complementary strategies for infection control and wound recovery. PEG-based polymer network covalently tethered with polyimidazolium (PIM) for contact-active biofilm eradication, and N-acetylcysteine (NAC) for antioxidative wound healing support, demonstrated complete killing of Methicillin-resistant S. aureus, P. aeruginosa, Carbapenem-resistant P. aeruginosa, and Carbapenem-resistant Acinetobacter baumannii in one hour.51 In diabetic mouse wounds, coated dressings achieved >3-log of bacteria, accelerated re-epithelialization and promoted granulation tissue formation compared to commercial silver dressings.
Garay-Sarmiento et al. introduced a Kill&Repel ultrathin wound dressing coating that combines antibiofouling polymer brushes with a contact-killing bactericidal enzyme, endolysin (EndLys).76 The antibiofouling component, N-(2-hydroxypropyl) methacrylamide (HPMA) and (3-methacryloylamino-propyl)-(2-carboxy-ethyl) dimethylammonium carboxybetaine methacrylamide (CBMAA), were grafted to a surface-affine fusion protein, forming a hydration-layer brush that reduced protein fouling from human plasma by up to 100%, fibroblast adhesion by >90%, and bacterial colonisation by E. coli by nearly 100%. EndLys hydrolysed the peptidoglycan layer of Streptococcus agalactiae (S. agalactiae) upon contact, achieving 92% killing of planktonic cells within 1 hour and 96% clearance of sessile bacteria on infected agar surfaces. To understand the performance of the immobilised EndLys, they evaluated the enzymatic cleavage of a FRET peptide substrate, showing that co-immobilised EndLys retained and even enhanced activity compared to the free enzyme, despite being present at a lower molar concentration (Fig. 6(a)). The immobilised enzyme achieved a 92% reduction in S. agalactiae planktonic cells after 1 hour of incubation, whereas the free enzyme at 1–2 μM only achieved 41–52% reduction (Fig. 6(b)). SEM imaging confirmed minimal bacterial attachment on the coated mesh after incubation in dense S. agalactiae suspensions (Fig. 6(c)). This non-leaching, non-toxic coating was stable for over 6 months and preserved biocompatibility in both extract and direct contact assays.
![]() | ||
| Fig. 6 Dual-functional performance of the Kill&Repel coating. (a) Schematic of the enzymatic activity assay using a peptide substrate labelled with aminobenzoyl (Abz, a fluorophore) and dinitrophenyl (Dnp, a quencher), enabling Förster Resonance Energy Transfer (FRET). Cleavage of the substrate by immobilised EndLys disrupts FRET and restores fluorescence. Fluorescence increase over time confirms the enzymatic activity of immobilised EndLys on pHPMA792/EndLys-coated meshes compared to free EndLys and control. (b) Illustration of localised bacterial killing by immobilised EndLys on the coating versus dispersed free EndLys. Quantification shows a 92% reduction in S. agalactiae concentration after 1 h with coated mesh, exceeding the efficacy of free EndLys at 1–2 μM. (c) SEM and fluorescence overlay images show markedly reduced bacterial adhesion (purple spots indicate bacteria) on coated polycaprolactone (PCL) mesh versus bare PCL. Scale bars are 10 μm. Reproduced with permission from ref. 76. Copyright 2022 John Wiley and Sons. | ||
Recent efforts have further explored the use of imidazolium-based zwitterionic polymers and biocompatible nanosilica composites. Chen et al. (2022) introduced a zwitterionic coating synthesised via initiated chemical vapour deposition (iCVD), a solvent-free, substrate-independent technique that enables uniform and conformal coating on complex surfaces (Fig. 7(a)).52 The process involved copolymerisation of vinyl imidazole and divinylbenzene via iCVD, followed by vapor-phase derivatization with 1,3-propanesultone to convert imidazole moieties into imidazolium sulfonate groups (Fig. 7(b)). This approach preserved the topographical integrity of diverse substrates, including curved 96-well plates (Fig. 7(c)), glass fibre filters with micrometre-scale 3D structure (Fig. 7(d)), and nanoporous membranes (Fig. 7(e)). SEM-EDX confirmed the presence of sulphur exclusively on coated surfaces. Functionally, the coating reduced coronavirus infectivity by 74%, viral adhesion by 97.4%, and bacterial biofilm formation to 15% of that on conventional polyvinyl chloride (PVC), while inhibiting pyoverdine production in P. aeruginosa biofilms by 67%.
![]() | ||
| Fig. 7 Synthesis and substrate versatility of the iCVD-derived zwitterionic coatings. (a) Schematic of iCVD setup and (b) post-deposition derivatization with 1,3-propanesultone. Conformal coatings were demonstrated on (c) curved 96-well plates, (d) micrometre-scale glass fibre filters, and (e) nanoporous membranes. Coatings preserved substrate morphology and showed sulphur presence only on treated surfaces. Reproduced with permission from ref. 52. Copyright 2022 The American Association for the Advancement of Science. | ||
| Dual-functional material | Contact angle | Zeta potential | Coating technique/surface texturing | Antimicrobial activity comes from | Antibiofouling activity comes from | Biocompatibility | Stability |
|---|---|---|---|---|---|---|---|
| Contact surface coatings | |||||||
| Imidazolium-based zwitterionic polymer52 | 9.9° ± 2.1° | −13 mV in a 100 mM NaCl standard solution at pH 7 | iCVD | Positively charged carbon atom at the C2 position | Strong electrostatic interaction with water molecules | — | Durable and insoluble in aqueous environments due to the incorporation of divinylbenzene as a cross-linker |
| AMP137 | 40.7° ± 1.8° | — | Dopamine-assisted modification | AMP | AMP | Non-toxic and environmentally friendly. | Maintained antibiofouling performance after immersion in artificial seawater for up to 21 days |
| MDPB/SBMA/polyurethane45 | 21.2 ± 4.3° | — | 3D printing | QA in MDPB | SBMA | Cell viability remaining >90% after 7 days of testing. | — |
| Nanosilica resin/AgNPs/TEGO®Addibit EK 5068 | 15.05° | — | Sol–gel transformation | AgNPs | Nanosilica resin and TEGO® Addibit EK 50 | Excellent biocompatibility | Abrasion resistance (2000 cycles), water resistance (72 hours), and aging resistance (48 hours UV exposure) |
| Food-related coatings | |||||||
| Gelatin/soy protein hydrolysate/tannic acid@low-density polyethylene (gel/SPH/TA@LDPE)36 | ∼30° | — | Atmospheric plasma treatment, solvent casting and crosslinking, chlorination | N-Halamine structures | Hydrophilicity | Do not exhibit cytotoxic effects | Retained 88.2% of its initial mass after 2 hours and 80.4% after 24 hours of water immersion. |
| Reduction: Listeria innocua 99.999%, E. coli 99.998% | |||||||
| Maintained 704 ppm active chlorine after 5 recharging cycles | |||||||
| Ag-coordinated poly(methacrylic acid) (Ag-PMAA)135 | 62.9 ± 2.0° | — | iCVD | Surface-bound Ag+ | Surface-bound Ag+ (non-leaching, contact-kill) | 97.4% viability of HDFa (vs. 8% on control PVC) | No measurable Ag+ leaching after 24 h; robust under immersion |
| Marine and water treatment | |||||||
| Carbonyl iron particles/silicone elastomer/ZIF-8/BNN6/methyl fluoro–silicone oil74 | ≈105° | — | Magnetic field self-assembly | Nitric oxide release under UV | Fluoro–silicone oil | — | Maintained its structure after 1000 bending cycles, with no significant degradation after 30 days in seawater |
| Carboxymethyl chitosan–zinc oxide/fluorinated polyurethane (CMC-ZnO/FPU)37 | 69° | — | Solution casting and curing at 60 °C for another 24 hour | UV-induced hydroxyl radicals and ROS from ZnO. electrostatic interactions with chitosan. survival rate- E.coli 3.14%, S. aureus- 2.53% | FPU | — | Withstanding temperatures up to 400 °C, maintaining structural integrity and performance after 30 days in stationary seawater and 14 days in flowing seawater |
| g-C3N4 nanosheet/poly-Schiff base composite coating (DPC-x)72 | Before degradation: 97.82°, after 5 days of immersion: 58.4°, after 50 days of degradation: 58.4° | g-C3N4 nanosheets: −18 mV in water | Solution casting | Photocatalytic activity of g-C3N4 nanosheets kills 99.31% in the dark and 99.87% in visible light. | Poly-Schiff base resin degrades to expose fresh g-C3N4 nanosheets, maintaining an active surface. | Environmentally friendly and non-toxic | — |
| Hydrophilic surface and negative zeta potential repel microorganisms. | |||||||
| α-lipoic acid QAS/ethylene glycol/lithium phenyl-2,4,6-trimethylbenzoylphosphinate48 | — | — | Drop casting | QAS >99.9% of S. aureus inactivation | Lithium phenyl-2,4,6-trimethylbenzoylphosphinate degrades with UV, exfoliating biofilm from the surface | Reduced toxicity | Maintain dual functional properties over multiple cycles |
| Mesoporous silica nanoparticles/QAS/DCOIT49 | 96° | n/a | Mixed with biocide-free paint and coated PVC panels | QA | DCOIT | Low toxicity to non-target species | — |
| Polylysine/tannic acid/poly(2-diisopropylaminoethyl methacrylate)-b-poly(2-methacryloyloxyethyl phosphorylcholine) (PLYS/TA/PDPA-b-PMPC)60 | 32° at pH 7.4, 24° at pH 5.5 | 2.7 mV at pH 7.4 | Immersion coating | PLYS chains −77% inhibition of adhered S. epidermidis | PMPC reduce bacterial adhesion to 22% | 90% cell viability | Stable over 30 days of immersion in filtered seawater & 14 days of exposure to flowing seawater at 13 cm s−1 |
| Houttuynia and scutellarin extracts blended with methylphenyl silicone resin (MSR)77 | >130° | — | Dip-coating | Bioactive compounds in houttuynia and scutellarin. Ex: decanal and safrole, which can disrupt bacterial cell walls and membranes | MRS provides low surface energy, making it difficult for fouling organisms to attach to the surface | — | Reduction rate after 30 days of seawater immersion – Houttuynia/MSR: 73.9% (E. coli), 99% (S. aureus) |
| Scutellarin/MSR: 91.3% (E. coli), 72.4% (S. aureus) | |||||||
| Houttuynia/MSR: 56.25% (Algae) | |||||||
| Scutellarin/MSR: 64.81% (algae) | |||||||
| Gel/GMTA/QA46 | — | +50 mV (pH 3–10) | Single-step grafting | QA-98% removal of E. coli from dairy wastewater | GMTA | Low cytotoxicity | Retains its viscosity and zeta potential after being stored at 4 °C for 10, 20, and 30 days |
| L-tryptophan/picolinic acid/4-nitrophenyl-isothiocyanate@AgNPs (gel@AgNPs)70 | 140 ± 2.0° | — | Self-assembly | AgNPs reduced viability by ∼95% in 4 hours against E. coli and S. aureus | Superhydrophobic organogel repels bacteria. | Do not inhibit cell proliferation at the tested concentrations | Strong resistance to external shear forces. |
While several dual-functional coatings demonstrate excellent performance in marine environments, their long-term environmental impact raises concern. For instance, a mesoporous coating composed of silica nanoparticles, QAS and 4,5-dichloro-2-octyl-4-isothiazolin-3-one (DCOIT) achieved 99% bacterial inhibition and only 6.9% surface fouling after six months.49 However, their reliance on biocide leaching, particularly DCOIT, poses risks of ecotoxicity. In contrast, biodegradable plant-derived coatings using Houttuynia and Scutellarin extracts showed up to 99% bacterial reduction and 35.92% less fouling in marine field tests.77 Polymer-based systems, such as the pH-responsive PDPA-b-PMPC/PLYS coating,60 offer biocide-free, switchable functionality and maintain performance over 30 days in static and 14 days in flowing seawater. Similarly, dopamine-assisted antimicrobial peptide coatings on stainless steel significantly reduced marine organism adhesion (>90%) via electrostatic disruption, without inducing toxicity in zebrafish or human renal cells.137 At the forefront, a chiral metal–organic framework coating (MPN-DMOF) assembled via Cu2+-mediated mineralisation of D-methionine on a tannic acid–polyethylenimine (TA–PEI) metal–polyphenol network demonstrated robust dual-functionality by integrating mechanical biofilm disruption with catalytic ROS generation.106 The synthesis process (Fig. 8(a)) involves sequential deposition of a uniform MPN adhesive layer (Fig. 8(b) and (c)), which facilitates stable and substrate-independent MOF growth. Subsequent mineralisation yields conformal microspheres with petal-like nanostructures (Fig. 8(d) and (e)), which are critical for exerting mechano-bactericidal effects by inducing membrane rupture through nanoscale protrusions and restricted bacterial adhesion. The multifunctional action of the coating (Fig. 8(f)) causes mechanical disruption, Cu2+-driven chemodynamic killing, D-amino-acid-mediated biofilm disassembly, and fluorescence-assisted algae repellence. Functionally, MPN-DMOF achieved a 5.6-log reduction of Bacillus vietnamensis biofilms, >91% E. coli membrane rupture, and further CFU reductions in P. aeruginosa and S. aureus, outperforming its L-methionine analogue in biofilm dispersal and gene-level suppression. The coating also demonstrated consistent wettability across diverse substrates and sustained Cu2+ release at 8.5 μg·cm−2 per day. Extending beyond marine use, Peng et al. introduced a non-leaching, energy-independent coating of carbon-coated Cu(OH)2 nanotips on copper foam that achieved >99.9% bacterial inactivation through physical rupture over 30 days.138
![]() | ||
| Fig. 8 Fabrication and functional mechanisms of a chiral MOF-based dual-functional coating. (a) Synthesis of the coating via metal–polyphenol network (MPN)-assisted mineralisation using tannic acid (TA), polyethylenimine (PEI), Cu2+, and D-methionine. (b), (c) SEM and AFM images showing uniform MPN anchoring on stainless steel. (d), (e) SEM images revealing conformal MOF microspheres with petal-like morphology. (f) Schematic illustration of the dual-functional mechanism, integrating mechano-bactericidal effects, Cu2+-driven chemodynamic killing, D-amino-acid-induced biofilm disassembly, and fluorescence-mediated algae inhibition. Reproduced with permission from ref. 106. Copyright John Wiley and Sons 2024. | ||
In this context, cellulose, the most abundant natural biopolymer, presents a compelling alternative.141 Cellulose, first isolated by Anselme Payen in 1838, has become a focus of extensive research due to its renewability, biodegradability, and surface reactivity.142,143 Among cellulose-based materials, nanocellulose (NC) has gained significant attention due to its unique combination of sustainability, low density, high aspect ratio, high crystallinity, strong hydrophilicity and a modifiable surface that enables tailored functionalisation.144 In addition, NC-based materials are compatible with scalable, low-cost application methods such as spray coating, facilitating their translation to industrial and biomedical settings.145,146 There are three main classes of NC: cellulose nanocrystals (CNCs), cellulose nanofibers (CNF), and bacterial nanocellulose (BNC), classified according to their morphology and source.147 Readers are advised to refer to Thomas et al.147 for an in-depth overview of NC, production methods, surface modifications, and application potential across diverse fields.
The earliest reported form of NC is acid hydrolysed CNCs which dates back to 1947.148 In 1949, these materials were referred to as “cellulose micelles and crystallites”.149 However, it was not until 1953 that electron micrograph imaging revealed that CNCs do not exist in a micelle form but instead exhibit a rod-like structure.150 Later in 1970, the term ‘Nanocellulose’ came into existence, which is now the standard term.151 A significant milestone came in 1983 when Turbak et al. developed CMFs through high-shear mechanical treatment of wood pulp, marking the precursor to CNFs.152 In the 1990s and 2000s, researchers like Akira Isogai153,154 advanced CNF production techniques. In 2011, the growing interest in NC led to the establishment of the first and world's largest CNC producer (1 ton per day), CelluForce® in Canada.155 Today, there are several other industrial-scale NC producers such as Alberta Innovates Technology Futures, Anomera Inc., GranBio and Forest Products Laboratories (supplied by the University of Maine).156,157
NC has shown potential for antibiofouling applications, as its hydrophilic surface prevents microbial adhesion and biofilm formation.158 For instance, NC coatings applied to polyethersulfone membranes reduced surface roughness from 30.5 nm to 4.7 nm for CNC and 7.6 nm for CNF, resulting in 49% less BSA protein adhesion and significantly reducing E. coli coverage to 0.2% compared to 10.2% on uncoated membranes.159 However, native NC lacks intrinsic antimicrobial activity160 and thus does not fulfil the criteria for dual-functionality. To address this limitation, recent studies have explored strategies to impart antimicrobial properties to NC while retaining its antibiofouling characteristics. First, surface hydroxyl groups can be chemically transformed into reactive moieties such as aldehydes with intrinsic antimicrobial activity.17 Second, antimicrobial compounds may be covalently grafted onto the NC to ensure stable, contact-active performance.161 Third, NC can serve as a template for the immobilisation of metal nanoparticles, which confer sustained microbial inhibition via surface-mediated interactions without uncontrolled release.162
We recently explored the dual-functional surface coating potential of dialdehyde cellulose microfibres (DACMF) derived from sugarcane trash (Fig. 9).17 The DACMF coating achieved 99% inactivation of S. aureus within 20 minutes (Fig. 9(a)), over 90% inhibition of E. coli within 60 minutes (Fig. 9(b)), and >99.9% reduction of influenza A/H1N1 virus just after 15 minutes of contact (Fig. 9(c)). Additionally, hydrophilic porous fibre architecture promotes hydration-mediated low fouling, while the aldehyde functionalities lead to irreversible inactivation of any adhered pathogens (Fig. 9(g)–(l)). Covalent grafting has also proven effective in enhancing the dual-functional properties of NC. For example, poly(sulphobetaine methacrylate) (PSBMA) grafted onto CNC reduced protein adsorption and achieved measurable antibacterial activity compared to no activity for pristine CNC.161 Similarly, grafting epoxy propyl dimethyl dodecyl ammonium chloride onto cellulose acetate membranes improved water permeability by 139% and flux recovery by 21.5%, while maintaining >99.99% inactivation of S. aureus and E. coli even after four antibacterial cycles, indicating long-term stability and durability.127 The negatively charged surface functionalities of NC (–OH, –COOH, SO42−) facilitate strong electrostatic interactions with metal ions, enabling effective templating and immobilisation of nanoparticles while preventing aggregations. This anchoring improves coating stability and promotes uniform nanoparticle distribution, enhancing antimicrobial performance while mitigating cytotoxicity through controlled release.70 For instance, silver nanoparticles templated CNCs (CNC/Ag) reduced adhesion of E. coli and B. subtilis by over 99%, compared to 66.9% and 32.9% with pristine CNCs and inactivated planktonic cells, with MIC values of 25 μg mL−1 for B. subtilis and 100 μg mL−1 for E. coli.162
![]() | ||
| Fig. 9 Dual-functional performance of dialdehyde cellulose (DAC) coatings. CMF: cellulose microfibres, DACMF: dialdehyde cellulose microfibres and DACNF: dialdehyde cellulose nanofibers. Time-dependent antibacterial activity of uncoated and coated surfaces against (a) S. aureus and (b) E. coli. (c) Antiviral efficacy. SEM images of bacterial accumulation and adhesion after 12 h of incubation: (d)–(j) uncoated, (e)–(k) CMF, and (f)–(l) DACMF-coated surfaces. Scale bar: 10 μm. Reproduced with permission from ref. 17, Copyright 2025 American Chemical Society. | ||
While nanocellulose offers promising features for dual-functional coatings, several challenges must be addressed to enable broader industrial adoption. One major limitation is its hydrophilic surface, which reduces compatibility with hydrophobic matrices, often requiring chemical modification that can increase cost and reduce sustainability. Achieving stable, homogeneous dispersion in different formulations is also difficult, as nanocellulose tends to aggregate or gel over time. Industrial-scale production is progressing, with ongoing challenges in achieving energy-efficient and low-chemical extraction methods.163,164 In particular, drying nanocellulose without compromising its structure and performance remains a significant hurdle. Conventional drying methods are energy-intensive, and once dried, nanocellulose is often difficult to rehydrate uniformly, which limits its processability and application flexibility. Nanocellulose's hydrophilicity supports antibiofouling yet can compromise dimensional stability under humid conditions and contributes to inconsistent hydration layer formation, an aspect critical for antifouling yet often under-characterised.165,166 Addressing these technical challenges is essential for unlocking the full potential of nanocellulose in sustainable coating technologies.
In addition to nanocellulose, chitosan- and protein-based surface coatings offer substantial potential as materials capable of inhibiting bacterial colonisation and preventing biofouling. The biopolymer's innate cationic nature facilitates electrostatic interactions with negatively charged microbial membranes, thereby disrupting cellular integrity and limiting biofilm formation. Functionalisation strategies such as PEGylation and nanoparticle incorporation have been shown to enhance chitosan's hydrophilicity and surface uniformity, effectively reducing bacterial adhesion and promoting long-term antifouling efficacy.167 Recent research has further demonstrated that tuning the surface roughness and chemical structure of chitosan-based films markedly improves their bactericidal performance while maintaining material stability.168 Mechanistic investigations have elucidated how chemical modifications, such as QA substitution and metal ion chelation, can significantly amplify chitosan's intrinsic antibacterial properties.169 In addition, chitosan-grafted microsphere systems can effectively enable controlled biocide release while maintaining low toxicity, highlighting a promising pathway toward sustainable high-performance dual-functional coatings.170 However, chitosan-based coatings can benefit from further optimisation in water stability and mechanical robustness under varying pH and in humid environments.171 Its incompatibility with hydrophobic surfaces often requires chemical modification, while dip-coated films commonly suffer from non-uniformity and limited durability.171,172
Protein-based surface coatings offer precise molecular architecture, inherent biocompatibility, and modular design capable of combining fouling-resistant, adhesive, and antimicrobial domains in single constructs. For instance, triblock proteins integrating zwitterionic peptides, mussel-adhesive sequences, and silver-binding motifs have demonstrated both antifouling and bactericidal actions.173 However, Protein-based coatings require cost-effective, scalable synthesis and greater enzymatic durability.174 Another key constraint is their structural instability, particularly under fluctuating temperature and humidity, which accelerates denaturation and compromises long-term antimicrobial efficacy.175,176 Additionally, integration with synthetic or hydrophobic substrates often necessitates cross-linking agents or chemical modifications, which can diminish their biodegradability and introduce cytotoxic residues.177 Furthermore, batch variability and susceptibility to microbial degradation pose additional challenges to standardization and shelf stability.178
Zinc-coordinated polydopamine coatings (PDA/Zn) offer a robust synthetic platform for dual-functional performance.179,180 A PDA/Zn surface, formed via one-pot dopamine polymerisation in zinc ammonium solution, exhibited superhydrophilicity and effectively inhibited the attachment of biological substances, including platelets and bovine serum albumin, while demonstrating antibacterial activity against E. coli and S. aureus through Zn2+–protein interactions without inducing cytotoxicity to mammalian cells.179 Building on this, a superamphophilic antimicrobial membrane incorporating a PDA/Zn metallo–polymeric framework on polyethylene terephthalate (PET) non-woven fabric enabled gravity-driven dehydration of aviation fuel, reducing water content below 10 ppm, and achieved near-complete bacterial eradication through Zn2+-mediated toxicity and mechanical puncture from nanostructure cusps.180 These PDA/Zn systems provide scalable alternatives, but should be evaluated for long-term biosafety and environmental impact due to potential ion leaching.
Despite significant progress, current approaches remain limited by antimicrobial agent leaching, short functional lifespans, cytotoxicity risks, and complex fabrications. Moreover, the overwhelming focus on antibacterial targets has left viral and fungal threats comparatively underexplored. This is a critical gap, given that viral infections account for millions of deaths annually,181 and fungal diseases affect over 6 million people each year, resulting in approximately 3.75 million deaths, of which 2.55 million are directly attributed to that fungal infection.182
As we move toward a “One Health” paradigm seeking to balance human, animal, and environmental health,183 future coatings must prioritise not only antimicrobial efficacy but also sustainability, durability, translational feasibility, and safety. In this broader context, NC emerges as a compelling material platform due to its abundance, biodegradability, surface tunability, and excellent mechanical properties. Alongside NC, other emerging systems such as chitosan, protein, and PDA/Zn hybrids offer versatile, biocompatible pathways toward dual-functional performance. We believe that coatings built on such sustainable and adaptable platforms can transition from reactive disinfection tools to proactive, scalable defences against diverse and evolving microbial threats.
| This journal is © The Royal Society of Chemistry 2025 |