AbstractMaterials with synchronous capabilities of color change and actuation have prospects for application in biomimetic dual-stealth camouflage and artificial intelligence. However, color/shape dual-responsive devices involve stimuli that are difficult to control such as gas, light or magnetism, and the devices show poor coordination. Here, a flexible composite film with electrochromic/actuating (238° bending angle) dual-responsive phenomena, excellent reversibility, high synchronization, and fast response speed (< 5 s) utilizes a single active component, W₁₈O₄₉ nanowires. From in situ synchrotron X-ray diffraction, first principles calculations/numerical simulations, and a series of control experiments, the actuating mechanism for macroscopic deformation is elucidated as pseudocapacitance-based reversible lattice contraction/recovery of W₁₈O₄₉ nanowires (i.e. nanostructure change at the atomic level) during lithium ion intercalation/de-intercalation. In addition, we demonstrate the W₁₈O₄₉ nanowires in a solid-state ionic polymer-metal composite actuator that operates stably in air with a significant pseudocapacitive actuation.