Jingteng Zhao, Zhongqiang Wang, Cong Tian, Huang Xiao, Jian Gao, Xin Cheng, Congying Song, Fang Li, Guoxing Li
Abstract Solid polymer electrolytes (SPEs) face critical limitations in ionic conductivity, ion transference numbers, and recyclability. We report a recyclable Turing‐structured polymer electrolyte (TPE) prepared at gas/liquid/solid interface through evaporation/diffusion‐driven instability. The Turing structure provides fast ion‐conduction surfaces/channels with periodic lithium (Li)‐ion (Li + ) self‐concentration domains to enable a 3D percolating Li + conduction, reducing migration barriers to achieve a high Li + conductivity (1.6 × 10 −3 S cm −1 at 25 °C) and transference number (0.61). TPEs enable stable cycling performance in various solid‐state batteries at low‐temperature conditions (−20 °C), alongside excellent self‐healing, flame‐retardant, and recyclable properties. Closed‐loop recycling recovers 86.5% of polymer precursors and 82.6% of costly Li bis(trifluoromethanesulfonyl)imide (LiTFSI) salt, with regenerated electrolytes retaining their initial performance. These results highlight the potential of Turing structure as a scalable design paradigm for sustainable and high‐performance energy storage and conversion systems.