Biological materials relied on multiple synergistic structural design elements typically exhibit excellent comprehensive mechanical properties. Hierarchical incorporation of different biostructural elements into a single artificial material is a promising approach to enhance mechanical properties, but remains challenging. Herein, a biomimetic structural design strategy is proposed by coupling gradient structure with twisted plywood Bouligand structure, attempting to improve the impact resistance of ceramic‐polymer composites. Via robocasting and sintering, kaolin ceramic filaments reinforced by coaxially aligned alumina nanoplatelets are arranged into Bouligand structure with a gradual transition in filament spacing along the thickness direction. After the following polymer infiltration, biomimetic ceramic‐polymer composites with a gradient Bouligand (GB) structure are eventually fabricated. Experimental investigations reveal that the incorporation of gradient structure into Bouligand structure improves both the peak force and total energy absorption of the obtained ceramic‐polymer composites. Computational modeling further suggests the substantial improvement in impact resistance by adopting GB structure, and clarifies the underlying deformation behavior of the biomimetic GB structured composites under impact. This biomimetic design strategy may provide valuable insights for developing lightweight and impact‐resistant structural materials in the future.

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