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Abstract Zn‐based solid polymer electrolytes (SPEs) have enormous potential in realizing high‐performance zinc‐ion batteries. Polymeric single‐ion conductor (PSIC)‐based SPEs can largely eradicate anion migration and side reactions of electrodes with decreased polarization, but the ionic conductivity is still unsatisfactory due to the tight localized ion interactions and sluggish chain motion. Herein, by employing the heterocyclic tetrazole as the anionic center of the side chain, a novel PSIC is fabricated with optimized charge delocalization and enhanced side‐chain motion. The as‐prepared PSIC delivers an ionic conductivity up to 5.4 × 10 −4 S cm −1 with an ultrahigh Zn 2+ transference number of 0.94. Based on the PSIC, dendrite‐free and hydrogen‐free Zn plating/stripping cycling (2000 h) is achieved. A further assembled Zn‖V 2 O 5 battery exhibits superior performances to other solid ZIBs, including a high discharge capacity, excellent rate capability, and long cycling life. In addition, a remarkable shelf‐life (90 d), low self‐discharge rate, and good temperature adaptability of the solid battery can be achieved benefiting from the high stability of the SPE during operation. The PSIC‐based SPEs with advanced ion‐transport structure endow solid ZIBs with significant performance improvement, high safety, and durability.
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