Wide‐Spectrum‐Tunable and Shape‐Reconfigurable Cholesteric Liquid Crystal Elastomers With a Continuous Pitch Gradient

ABSTRACT Achieving synchronous opto‐mechanical regulation of the elastomers inspired by the communication and survival strategies of living organisms is highly desirable but remains challenging, due to the difficulty of homogeneous periodic structures in generating the asymmetric strains required for mechanical deformation. Herein, we report a nanowire assembly‐directed hierarchical structuring strategy for fabricating spectrally tunable and solvent‐adaptive structural color actuators with continuous gradient helices embedded in an anisotropic framework via an asynchronous photopolymerization. Arising from spatially continuous modulated photonic structure, the obtained film enables a wide‐spectrum color gamut with high‐purity photonic outputs tuning from 380 to 756 nm through dopant‐nanowire assembly coregulation, beyond that of the reported photonic materials. Upon differentially regulating cholesteric periodicity in varied solvents, the composite undergoes rapid, reversible optical shifts across 380–703 nm within 3 s. Moreover, solvent‐induced asymmetric swelling releases internal stress that induces shape reconfiguration with inverse chirality accompanied by photonic transition, which produces directional 3D rotation with vivid color change when assembled into a windmill actuator. Thus, this hierarchically engineered CLCE platform offers a robust foundation for designing environmentally adaptive photonic devices.