Inspired by nature, diverse biomimetic hydrogel actuators have been fabricated and become one of the most essential components of bionics research. Usually, the anisotropic structure of a hydrogel actuator is generated at the early fabrication process, only a specific shape transformation behavior could be produced under external stimuli, and thus has limited the development of hydrogel actuators toward the biomimetic shape deformation behavior. Herein, we propose a novel bilayer hydrogel having a thermo-responsive actuating layer and a metal ion-responsive memorizing layer, therefore, a 2D hydrogel film can be fixed into various 3D shapes via supramolecular metal-ligand coordination, with further realizing programmable 4D shape deformation under the stimulus of temperature. By manipulating the temporary shapes via shape memory behavior, various temporary anisotropic structures could be obtained via the bilayer hydrogel, thus producing diverse reversible shape deformation performances, which is expected to promote the development of intelligent polymeric materials.