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The instability of Li10GeP2S12 toward moisture and that toward lithium metal are two challenges for the application in all‐solid‐state lithium batteries. In this work, Li10GeP2S12 is fluorinated to form a LiF‐coated core–shell solid electrolyte LiF@Li10GeP2S12. Density‐functional theory calculations confirm the hydrolysis mechanism of Li10GeP2S12 solid electrolyte, including H2O adsorption on Li atoms...