Intensive exploration and research in the past few decades on polysaccharide nanocrystals, the highly crystalline nanoscale materials derived from natural resources, mainly focused originally on their use as a reinforcing nanophase in nanocomposites. However, these investigations have led to the emergence of more diverse potential applications exploiting the functionality of these nanomaterials. Based on the construction strategies of functional nanomaterials, this article critically and comprehensively reviews the emerging polysaccharide nanocrystal-based functional nanomaterials with special applications, such as biomedical materials, biomimetic optical nanomaterials, bio-inspired mechanically adaptive nanomaterials, permselective nanostructured membranes, template for synthesizing inorganic nanoparticles, polymer electrolytes, emulsion nano-stabilizer and decontamination of organic pollutants. We focus on the preparation, unique properties and performances of the different polysaccharide nanocrystal materials. At the same time, the advantages, physicochemical properties and chemical modifications of polysaccharide nanocrystals are also comparatively discussed in view of materials development. Finally, the perspective and current challenges of polysaccharide nanocrystals in future functional nanomaterials are outlined.