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Water Processable Bioplastic Films from Functionalized Protein Fibrils

A combination of mechanochemistry and aqueous self‐assembly is employed to prepare protein nanofibrils (PNFs) functionalized with perylene diimide (PDI) dyes. These materials are then mixed with poly(vinyl alcohol) (PVA) and casted into bioplastic films. The functionalization process not only results in luminescent hybrid materials, but the presence of the dye modifies the physical properties of the PNFs. Films formed from PNFs functionalized with PDIs display anisotropic organization, which enables emission of polarized light. Crucially, the presence of PDI dyes improves the stability of PNF‐PVA films in water and moreover the films are processable when wet. By applying water, films can be glued together or self‐healed by applying water. Mechanochemical methodology can thus be employed for modifying properties of protein materials. This represents a new highly flexible and novel strategy for tuning both properties and functionality of protein materials.