<p>Lead-free barium titanate (BaTiO₃) nanofiber material is an attractive functional material. However, as a ceramic material, its inherent brittleness significantly limits its widespread application. Herein, we optimized the solution blow spinning process using aerodynamic simulations, enabling the efficient fabrication of layered barium titanate/aluminum oxide (BaTiO₃/Al₂O₃) ceramic nanofiber aerogels. The incorporation of amorphous Al₂O₃ repaired the defects in the nanofibers, providing aerogels with outstanding mechanical properties. For example, these aerogels can support nearly 1000 times their own weight, exhibit a tensile strain of 11%, and demonstrate exceptional compressive resilience and fatigue resistance. Additionally, the aerogels demonstrated superior performance in flexible electronics, thermal protection, sound absorption, and high-temperature filtration. This research paves the way for the large-scale production and extensive application of flexible piezoelectric ceramic aerogels.</p> Graphical abstract <p></p>