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Oxide perovskite ceramics are cornerstone materials of electronic devices, but they easily break under bending. Such brittle failure phenomenon limits their applications in emerging flexible electronics. Here, the authors propose a scalable approach of sol-gel electrospinning to synthesize flexible perovskite Li0.35 La0.55 TiO3 (LLTO) nanofibers (NFs) by reducing grain sizes and pore defects in the NFs. The strategy is to precisely control crystal nucleation and growth by forming homogeneous nuclei in the sol before electrospinning and