Programmable Liquid Crystal Elastomer‐Based Reconfigurable Rigid Foldable Origami Enabled by Hybrid Surface‐Induced Alignment

Rigid foldable origami, valued for its geometric programmability, load‐bearing capacity, and reconfigurability, is essential for applications in architecture, engineering, and biomedicine. Liquid crystal elastomer (LCE)‐based active origami offers reversible deformation, large actuation strain, and multi‐stimuli responsiveness but has been limited by alignment technology, hindering high‐resolution voxel‐to‐voxel alignment in 2D and vertical directions. Herein, a hybrid alignment strategy combining photoalignment and vertical polyimide (PI) alignment via a patterned mask is proposed, enabling precise molecular control in monolithic LCE films. This approach allows high‐resolution fabrication of voxel units in various forms, achieving precise control over folding patterns, curvature, angles, and kinetics. Several thermally and photo‐responsive LCE origamis in simulations and experiments are demonstrated, along with an LCE Miura‐ori‐based microwave metasurface that supports 46.8 times its weight and modulates microwave frequency and reflectance with 8.81 dB depth at 24.28 GHz. This strategy advances applications in biomimetic devices, deployable structures, and reconfigurable electromagnetic systems.