Bioinspired Strong and Tough Layered Bulk Composites via Mycelial Interface Anchoring Strategy

Abstract Lightweight structural composite materials are widely used in automobiles, aerospace, and other fields. However, achieving the integration of structural and functional properties, such as the ability to monitor external forces, remains a significant challenge. Nacre and turtle shells in nature are strong and tough due to their unique ordered structure of alternating soft and hard phases. Inspired by this, an interface anchoring strategy is proposed which leverages hyphae (filamentous structure forming the vegetative part of fungi) to fix the hard‐phase graphene nanosheets (GNs) and the soft‐phase intertwined polymer matrix to form theree‐dimentional (3D) layered bulk composites (LBCs). The growth pattern of fungi is utilized to place GNs and assemble polyethylene glycol‐polyvinyl alcohol (PEG‐PVA) to fabricate the LBCs, which is different from most existing preparation methods of bulk biomimetic composites. The LBCs exhibit self‐regenerative capabilities and are amenable to scalable manufacturing. These composites demonstrate impressive mechanical properties, including a specific strength of 92.8 MPa g cm −3 , fracture toughness of 6.5 MPa m −1/2 , and impact resistance of ∼3.1 kJ m −2 , outperforming both natural nacre and other biomimetic layered composites. Furthermore, the LBCs display effective protective warning functions under external force stimulations, making them a promising material for anti‐collision applications in industries such as sports and aerospace.