Liquid‐crystalline polymers with photodeformable properties have been extensively studied due to their ability of wireless conversion of light energy into mechanical work. With the development of crosslinked liquid‐crystalline polymers, various 3D motions, such as bending, twisting, oscillation, rotation, and translational motion have been successfully induced. Recent trends for developing soft robots and microrobots accelerate the progress of photomobile polymer materials. This review is focused on recent advances in the field of photomobile materials based on liquid‐crystalline polymers. The structure–function relationship in photomobile polymer materials is overviewed, and the progress in recent years is detailed in terms of complex 3D deformation, continuous motions, self‐regulation, and processability.