Fabrication of bioinspired intelligent materials with adjustable light, self-shading, and tunable color performances is a significant challenge in the fields of advanced materials. In this work, a liquid crystal nanoparticle actuator (LCNA) with photo-humidity stimuli responses was designed, which was supramolecular self-assembled by the surfactantassisted method from a functional liquid crystal molecule 2-(3′,3′-dimethyl-6-nitrospiro[chromene-2,2′-indolin]-1′-yl)ethyl dodecyl phthalate (EDP-SP). Bionic films containing the LCNA showed adjustable light, selfshading, and color changes in response to environmental light and humidity stimuli. The self-assembled amphiphilic nanoparticles greatly improved the stimuli-responsive sensitivity. A bionic nanoactuator was triggered by multiple supramolecular interactions, such as the rearrangement of liquid crystal molecules, the interactions of intermolecular hydrogen bonds, and the photoisomerization in the nanoparticles. They show excellent dimming and color-changing sensitivity and reversibility in real time. Bionic interfaces containing the self-assembled LCNA attract much interest and have many potential applications in 3D printing, smart textiles, and artificial bionic skin.