Abstract The combination of complex perception, defense, and camouflage mechanisms is a pivotal instinctive ability that equips organisms with survival advantages. The simulations of such fascinating multi‐stimuli responsiveness, including thigmotropism, bioluminescence, color‐changing ability, and so on, are of great significance for scientists to develop novel biomimetic smart materials. However, most biomimetic color‐changing or luminescence materials can only realize a single stimulus‐response, hence the design and fabrication of multi‐stimuli responsive materials with synergistic color‐changing are still on the way. Here, a bioinspired multi‐stimuli responsive actuator with color‐ and morphing‐change abilities is developed by taking advantage of the assembled cellulose nanocrystals‐based cholesteric liquid crystal structure and its water/temperature response behaviors. The actuator exhibits superfast, reversible bi‐directional humidity and near‐infrared (NIR) light actuating ability (humidity: 9 s; NIR light: 16 s), accompanying with synergistic iridescent appearance which provides a visual cue for the movement of actuators. This work paves the way for biomimetic multi‐stimuli responsive materials and will have a wide range of applications such as optical anti‐counterfeiting devices, information storage materials, and smart soft robots.