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Artificial muscles based on stimuli-responsive polymers usually exhibit mechanical compliance, versatility, and high power-to-weight ratio, showing great promise to potentially replace conventional rigid motors for next-generation soft robots, wearable electronics, and biomedical devices. In particular, thermomechanical liquid crystal elastomers (LCEs) constitute artificial muscle-like actuators that can be remotely triggered for large stroke, fast response, and highly repeatable actuations. Here, we introduce a digital light processing (DLP)–based additive manufacturing approach that automatically shear aligns mesogenic oligomers, layer-by-layer, to achieve high orientational order in the photocrosslinked structures; this ordering yields high specific work capacity (63 J kg −1 ) and energy density (0.18 MJ m −3 ). We demonstrate actuators composed of these DLP printed LCEs’ applications in soft robotics, such as reversible grasping, untethered crawling, and weightlifting. Furthermore, we present an LCE self-sensing system that exploits thermally induced optical transition as an intrinsic option toward feedback control. 

This article introduces a simple two‐stage method to synthesize and program a photomechanical elastomer (PME) for light‐driven artificial muscle‐like actuations in soft robotics. First, photochromic azobenzene molecules are covalently attached to a polyurethane backbone via a two‐part step‐growth polymerization. Next, mechanical alignment is applied to induce anisotropic deformations in the PME‐actuating films. Cross‐linked through dynamic hydrogen bonds, the PMEs also possess autonomic self‐healing properties without external energy input. This self‐healing allows for a single alignment step of the PME film and subsequent “cut and paste” assembly for multi‐axis actuation of a self‐folded soft‐robotic gripper from a single degree of freedom optical input.