Cucurbituril-assisted supramolecular polymeric hydrogels (CB-SPHs), formed by supramolecular cross-linking of polymer chains via directional noncovalent interactions, are a novel class of three-dimensional cross-linked polymeric materials with unique properties including stimuli responsiveness, processability, water-retention ability, biocompatibility, biodegradability, biostability, self-healing and shape-memory abilities. Cucurbit[n]urils (CB[n]) with rigid symmetrical structure and remarkably high binding affinity to guest molecules are commonly used macrocyclic hosts for SPHs. Due to the dynamic CB[n] host–guest interactions, CB-SPHs undergo reversible gel–sol conversion and can effectively change their physicochemical and mechanical properties upon exposure to external stimuli. These aqueous polymeric networks exhibit exceptional advantages in a wide variety of biomedical and industrial applications. This chapter describes the recent achievements in the design, synthesis and properties of CB-SPHs constructed through noncovalent interactions of CB[n] hosts with specific chemical motifs pendant from polymer chains, as well as their applications in various fields such as drug delivery, wound dressing and healing, tissue engineering, diagnostic devices, wood conservation, adhesives, stretchable and wearable electronics, injection and printing substances etc.