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The fillers in composite solid‐state electrolyte are mainly responsible for the enhancement of the conduction of Li ions but barely regulate the formation of solid electrolyte interphase (SEI). Herein, a unique filler of dielectric NaNbO3 for the poly(vinylidene fluoride) (PVDF)‐based polymer electrolyte, which is subjected to the exchange of Li+ and Na+ during cycling, is reported and the substituted...