The formation of surface-grafted polypeptide films and interfaces via N-carboxyanhydride ring-opening polymerization (NCA-ROP) holds great potential for the facile preparation of next-generation multifunctional and responsive materials with excellent biocompatibility, biodegradability, tunable conformations and chemical functionalities. Therefore, the aim of this feature article is to provide a topical review of developments in the area of polypeptide films derived through NCA-ROP. It is evident that studies reported thus far have only started to unveil the full potential of peptide-based interfaces and materials, and with continued advancements it is anticipated that the strategic combination of NCA-ROP with modern synthetic chemistries will continue to yield versatile platforms for broader applications in the fields of polymer therapeutics, tissue engineering, (bio)nanocoatings, (bio)chemosensors, catalysis and separation technologies.
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