the mantle of squids mainly comprises two groups of muscle fibers: the circumferential fibers that constitute the bulk of the mantle wall, and the radial fibers that are distributed in the mantle wall as to partition the circumferential ones. [2] Squids expand their mantle radially, filling the mantle cavity with water. Then the circumferential muscles contract, pushing the water out of the mantle cavity through the funnel. Repetition of these movements results in a pulsed jet. Inspired by these natural systems, there are many efforts devoted to developing soft active materials with anisotropic structures by hybridizing liquid crystals or nanoparticles. Anisotropic materials fulfill specific functions and enable various applications including mass transport, [3] structural colors, [4] actuations, [5,6] and soft robotics. [1a,b,7] In addition, programmable, complex ordered materials display local response under stimuli and show intriguing 3D configurations, imitating actuation or locomotion of living organisms. [6a,e,7c] Although photo-and surface-mediated molecular alignments are versatile to fabricate liquid crystalline elastomer/network films with distributed ordered structures. [6b,8] The thickness and dimensions of the films are usually limited in micrometer scale, and the strategy cannot be extended to other systems like hydrogels with sophisticated alignments. So far, preparation of anisotropic Living organisms use musculatures with spatially distributed anisotropic structures to actuate deformations and locomotion with fascinating functions. Replicating such structural features in artificial materials is of great significance yet remains a big challenge. Here, a facile strategy is reported to fabricate hydrogels with elaborate ordered structures of nanosheets (NSs) oriented under a distributed electric field. Multiple electrodes are distributed with various arrangements in the precursor solution containing NSs and gold nanoparticles. A complex electric field induces sophisticated orientations of the NSs that are permanently inscribed by subsequent photo-polymerization. The resultant anisotropic nanocomposite poly(N-isopropylacrylamide) hydrogels exhibit rapid deformation upon heating or photoirradiation, owing to the fast switching of permittivity of the media and electric repulsion between the NSs. The complex alignments of NSs and anisotropic shape change of discrete regions result in programmed deformation of the hydrogels into various configurations. Furthermore, locomotion is realized by a spatiotemporal light stimulation that locally triggers time-variant shape change of the composite hydrogel with complex anisotropic structures. Such a strategy on the basis of the distributed electric-field-generated ordered structures should be applicable to gels, elastomers, and thermosets loaded with other anisotropic particles or liquid crystals, for the design of biomimetic/ bioinspired materials with specific functionalities.