Despite extensive efforts to mimic the fascinating adhesion capability of geckos, the development of reversible adhesives underwater has long been lagging. The appearance of mussels-inspired dopamine chemistry has provided the feasibility to fabricate underwater adhesives; however, for such a system, imitating the reversible and fast dynamic attachment/detachment mechanism of gecko feet still remains unsolved. Here, by synthesizing a thermoresponsive copolymer of poly(dopamine methacrylamide-co-methoxyethyl-acrylate-co-N-isopropyl acryla-mide) and then decorating it onto mushroom-shaped poly(dimethylsiloxane) pillar arrays, a novel underwater thermoresponsive gecko-like adhesive (TRGA) can be fabricated, yielding high adhesion during the attachment state above the lower critical solution temperature (LCST) of the copoly mer, yet low adhesion during the detachment state below the LCST of the copoly mer. By integrating the Fe₃O₄ nanoparticles into the TRGA, TRGAs responsive to near-infrared laser radiation can be engineered, which can be successfully used for rapid and reversible remote control over adhesion so as to capture and release heavy objects underwater because of the contrast force change of both the normal adhesion force and the lateral friction force. It is also demonstrated that the material can be assembled on the tracks of an underwater mobile device to realize controllable movement. This opens up the door for developing intelligent underwater gecko-like locomotion with dynamic attachment/detachment ability.