Ceramic aerogels are often used when thermal insulation materials are desired; however, they are still plagued by poor mechanical stability under thermal shock. Here, inspired by the dactyl clubs of mantis shrimp found in nature, which form by directed assembly into hierarchical, chiral and Bouligand (twisted plywood) structure exhibiting superior mechanical properties, we present a compositional and structural engineering strategy to develop strong, superelastic and fatigue resistance ceramic aerogels with chiral fibers array resembling Bouligand architecture. Benefiting from the stress dissipation, crack torsion and mechanical reinforcement of micro-/nano-scale Bouligand array, the tensile strength of these aerogels (170.38 MPa) is between one and two orders of magnitude greater than that of state-of-the-art nanofibrous aerogels. In addition, the developed aerogels feature low density and thermal conductivity, good compressive properties with rapid recovery from 80 % strain, and thermal stability up to 1200 °C, making them ideal for thermal insulation applications.