In order to endow liquid crystal elastomers (LCE) with multiple-stimuli-responsiveness and enhance their potential application in flexible robotics, we developed an interfacial polymerization strategy to fabricate a bilayer nanocomposite LCE with photochemical, photothermal, and magnetic responsiveness. The Fe₃O₄ nanoparticles coated with octa-vinyl polyhedral oligomeric silsesquioxane (POSS@Fe₃O₄ NPs) were sprayed onto the surface of partially polymerized azobenzene LCE, and then induced the free radical polymerization between the unreacted acrylic-ester groups in the polymeric matrix and the abundant vinyl on the magnetic nanomaterials layer, to yield a POSS@Fe₃O₄ NPs-LCE composite (PFe-LCEs) with a tightly-integrated organic-inorganic interface. With merits of the UV-induced isomerization of azobenzene mesogens and the photothermal conversion capability of POSS@ Fe₃O₄ NPs, the composite elastomer could generate a 200° bending in 2 s under UV irradiation and returned to its initial state within 7.5 s under infrared light exposure. In contrast, utilizing visible light irradiation for 50 s can only restore 83% of the original shape. Additionally, this material exhibits magnetic responsiveness, allowing it to deflect under an applied magnetic field. The PFe-LCE was used to fabricate a quadrupedal transport robot capable of grasping, transporting, and releasing cargo through light-magnetic synergistic actuation in a complex environment. The demonstrated environmental adaptability highlighted a novel strategy for intelligent actuation in soft robotics.