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Solid-state electrolyte (SSE) is promising in next-generation lithium (Li) metal batterie (LMB) applications because of its significantly enhanced safety and more compatible interface characteristics than flammable, volatile traditional liquid electrolyte. Combining the strengths of inorganic solid-state electrolytes and solid-state polymer electrolytes, composite solid electrolytes (CSEs) are practically more viable for commercial applications. However, only a few efforts have achieved high-voltage (>4.3 V vs. Li/Li+) LMBs with distinguished comprehensive performance, which is mainly attributed to the fact that CSEs with both high ionic conductivity and good compatibility with electrodes are difficult to obtain. Furthermore, the relatively tedious fabrication process, such as the ex-situ solution casting technique accompanied by the use of noxious organic solvents, can hardly meet the practical needs of large-scale commercial production.