Nacre‐Mimetic Multi‐Mechanical Synergistic Ceramic Aerogels with Interfacial Bridging and Stress Delocalization

Abstract Elastic ceramic aerogels are exceptionally suitable for thermal insulating applications, but lacking multi‐mechanical synergistic high strength remains a deficiency. Inspired by the robust protective shells of mollusks in nature, which feature distinct hierarchical ordered structures, exhibiting strong and tough mechanical properties, a system construction and structural governing strategy is proposed to allow the nanostructure to assemble strong and flexible ceramic aerogels. Through the design of a hierarchical multi‐arched structure configurated binary‐soldering‐assemble interfacial topology interlocking, concentrated stress is effectively discrete. This biomimetic strategy enables the effective dissipation of mechanical energy, resulting in ceramic aerogels with exemplary compressive resilience, bendability, tensile resistance, and their strength exceeding that of other nanofibrous aerogels by up to tenfold. Additionally, the flexible aerogels also show remarkable thermal resistance from −196 to 1100 °C and superior thermal insulation capabilities (39.72 mW m⁻¹ K⁻¹), making them more suitable for the applications.