Protein micro/nanopatterning has long provided sophisticated strategies for a wide range of applications including biointerfaces, tissue engineering, optics/photonics, and bioelectronics. We present here the use of regenerated silk fibroin to explore wrinkle formation by exploiting the structure–function relation of silk. This yields a biopolymer-based reversible, multiresponsive, dynamic wrinkling system based on the protein’s responsiveness to external stimuli that allows on-demand tuning of surface morphologies and properties. The polymorphic transitions of silk fibroin enable modulation of the wrinkle patterns and, consequently, the material’s physical properties. The interplay between silk protein chains and external stimuli enables control over the protein film’s wrinkling dynamics. Thanks to the versatility of regenerated silk fibroin as a technological substrate, a number of demonstrator devices of varying utility are shown ranging from information encoding to modulation of optical transparency and thermal regulation.

Structurally colored materials, which rely on the interaction between visible light and nanostructures, produce brilliant color displays through fine control of light interference, diffraction, scattering, or absorption. Rationally combining different color‐selective functions into a single form offers a powerful strategy to create programmable optical functions which are otherwise difficult, if not impossible to obtain. By leveraging structural protein templates, specifically silk fibroin, nanostructured materials that combine plasmonic and photonic crystal paradigms are shown here. This confluence of function enables directional, tunable, and multiple co‐located optical responses derived from the interplay between surface plasmon resonance and photonic bandgap effects. Several demonstrations are shown with programmable coloration at varying viewing sides, angle, and by solvent infiltration, opening avenues for smart displays and multi‐mode information encoding applications.