Abstract Flexible materials with dynamic structural colors have attracted considerable interest for multilevel information interaction, showing great potential in visual interfaces, anti‐counterfeiting, and optical sensing. However, replicating 3D coupling of geometry and color found in nature, where shape morphing and optical modulation act together, remains a major challenge for soft materials. Herein, we report a stress‐guided photo‐programming strategy to encode multilevel 2D‐to‐3D information into cholesteric liquid crystal elastomers (CLCEs) through locally defined crosslinking networks. Specifically, spatially controlled UV exposure under programmed mechanical pre‐strain creates anisotropic crosslinking gradients, which locally lock in stress distributions and orient the cholesteric helix. The hierarchical stress of photochemical patterning and mechanical strain enables simultaneous 3D shape morphing and structural color evolution from a single 2D film precursor, constructing geometry‐color dual‐channel information carriers. The mechanical and optical programming are decoupled: internal laser‐defined crosslink gradients determine the cholesteric pitch, while external deformation drives geometric transformation. Consequently, hidden multi‐stage information can be visually decoded through programmable 3D deformation, encrypted patterns, and color transitions. This work establishes a generalizable paradigm for integrating stress‐driven mechanics and photonic functionality in soft materials, offering broad potential for dynamic encryption, multifunctional robotics, and interactive devices.
Wu et al. (Thu,) studied this question.