Exploring the interrelationships between microstructure, hydrophilicity, humidity response, and material stability through molecular structure design and low-cost preparation, and manufacturing sensing and driving materials with a perfect balance between structures and properties is crucial for biomimetic robots and intelligent devices. Herein, inspired by the capillary phenomenon, the cellulose nanofiber (CNF) was grafted by using taurine to form the “micro cilia” microstructure on its surface (CNF-TAU). By controlling the cilia density and symmetry, the hydrophilicity of the materials was adjusted, and the water was allowed to quickly separate from the inside of the materials, which led to improving the humidity sensitivity and stability of materials. Concretely, compared with CNF, the puncture load, tearing strength, and elongation at break of the CNF-TAU-1.0 were improved by 11.95 times, 2.16 times, and 15.6 %, respectively, and excellent tensile strength was presented. Moreover, the hydrophilicity of CNF-TAU was first weakened and then enhanced with TAU content increasing. At last, the CNF-TAU-1.0 (WCA 55.43°) was selected and blended with single-layer graphene oxide (GO) to prepare CNF-TAU/GO composite films by vacuum filtration. The results indicated that the composite film had excellent mechanical (room and high humidity), humidity responsiveness, and humidity gradient-driven properties. In detail, the CNF-TAU/GO-10 % composite film had the generated stable induced voltage (68.4 mV), the fast response/recovery time (0.3 s/0.9 s), the large max. bending angle (178.4°), and the drive cycle stability (1000 cycles). Moreover, the composite film could be applied to produce biomimetic soft robots, such as human fingers and butterfly-shaped robots.
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