Bioinspired smart materials with synergistic allochroic luminescence and complex deformation are expected to play an important role in many areas of science and technology. However, it is still challenging to fabricate such soft actuators with high programmability that can be manipulated in situ with high spatial resolution. Herein, we have incorporated terminally functionalized aggregation‐induced emission active tetraphenylethene derivative and photochromic spiropyran moieties into the networks of liquid crystal elastomers through covalent bonding to obtain the synergistic photochromic luminescence and programmable soft actuators. Bio‐mimic functions and light‐induced auxetic metamaterial‐like devices were shown to be feasible based on the combination of assembly and origami‐programming strategy. These bioinspired devices with synergistic photochromic luminescence and complex photodeformation abilities provide an elegant strategy to design multi‐functional liquid crystal actuators. Inspired by the synergic allochroic and shape‐morphing bio‐functions like caterpillars and cephalopods, photochromic luminescent liquid crystal actuators were prepared. Complex movements and fluorescent colors can be synergically manipulated by light based on the phase transition of liquid crystals and photoresponse of the fluorescent chromophores after the actuators were programmed with hybrid mesogenic alignments.