The strong interaction between graphene oxides (GO) and water molecules has trigged enormous research interest in developing GO‐based separation films, sensors, and actuators. However, sophisticated control over the ultrafast water transmission among the GO sheets and the consequent deformation of the entire GO film is still challenging. Inspired from the natural “quantum‐tunneling‐fluidics‐effect,” here quantum‐confined‐superfluidics‐enabled moisture actuation of GO paper by introducing periodic gratings unilaterally is reported. The folded GO nanosheets that act as quantum‐confined‐superfluidics channels can significantly promote water adsorption, enabling controllable and sensitive moisture actuation. Water‐adsorption‐induced expansion along and against the normal direction of a GO paper is investigated both theoretically and experimentally. Featuring state‐of‐the‐art of ultrafast response (1.24 cm−1 s−1), large deformation degree, and complex and predictable deformation, the smart GO papers are used for biomimetic mini‐robots including a creeping centipede and a smart leaf that can catch a living ladybug. The reported method is simple and universal for 2D materials, revealing great potential for developing graphene‐based smart robots.
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