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Composite polymer electrolytes (CPEs) are subject to interface incompatibilities due to the space charge layer of ceramic and polymer phases. The intensive dehydrofluorination of poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVDF‐HFP) incorporating Li7La3Zr2O12 (LLZO) significantly compromises electro‐chemo‐mechanical properties and compatibilities with electrodes. Herein, this study addresses...