Facile Anisotropic Deswelling Method for Realizing Large‐Area Cholesteric Liquid Crystal Elastomers with Uniform Structural Color and Broad‐Range Mechanochromic Response

Abstract Cholesteric liquid crystal elastomers (CLCEs) are soft and dynamic photonic elements that couple the circularly polarized structural color from the cholesteric helix to the viscoelasticity of rubbers: the reflection color is mechanically tunable (mechanochromic response) over a broad range. This requires uniform helix orientation, previously realized by long‐term centrifugation to ensure anisotropic deswelling, or using sacrificial substrates or external fields. The present paper presents a simple, reproducible, and scalable method to fabricate highly elastic, large‐area, millimeters thick CLCE sheets with intense uniform reflection color that is repeatably, rapidly, and continuously tunable across the full visible spectrum by stretching or compressing. A precursor solution is poured onto a substrate and allowed to polymerize into a 3D network during solvent evaporation. Pinning to the substrate prevents in‐plane shrinkage, thereby realizing anisotropic deswelling in an unprecedentedly simple manner. Quantitative stress–strain–reflection wavelength characterization reveals behavior in line with theoretical predictions: two linear regimes are identified for strains below and above the helix unwinding threshold, respectively. Up to a doubling of the sample length, the continuous color variation across the full visible spectrum repeatedly follows a volume conserving function of the strain, allowing the CLCE to be used as optical high‐resolution strain sensor.