Biomimetic Silk Architectures Outperform Animal Horns in Strength and Toughness

Structural biomimicry is an intelligent approach for developing lightweight, strong, and tough materials (LSTMs). Current fabrication technologies, such as 3D printing and two‐photon lithography often face challenges in constructing complex interlaced structures, such as the sinusoidal crossed herringbone structure that contributes to the ultrahigh strength and fracture toughness of the dactyl club of peacock mantis shrimps. Herein, bioinspired LSTMs with laminated or herringbone structures is reported, by combining textile processing and silk fiber “welding” techniques. The resulting biomimetic silk LSTMs (BS‐LSTMs) exhibit a remarkable combination of lightweight with a density of 0.6–0.9 g cm(−3), while also being 1.5 times stronger and 16 times more durable than animal horns. These findings demonstrate that BS‐LSTMs are among the toughest natural materials made from silk proteins. Finite element simulations further reveal that the fortification and hardening of BS‐LSTMs arise primarily from the hierarchical organization of silk fibers and mechanically transferable meso‐interfaces. This study highlights the rational, cost‐effective, controllable mesostructure, and transferable strategy of integrating textile processing and fiber “welding” techniques for the fabrication of BS‐LSTMs with advantageous structural and mechanical properties. These findings have significant implications for a wide range of applications in biomedicine, mechanical engineering, intelligent textiles, aerospace industries, and beyond.