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All‐solid‐state batteries (ASSBs) using sulfide electrolytes have attracted ever‐increasing interest due to high ionic conductivity of the sulfides. Nevertheless, a thin, strong solid‐state sulfide electrolyte membrane maintaining high ionic conductivity is highly desired for ASSBs. Here, a thin, flexible composite solid electrolyte membrane composed of argyrodite sulfide Li6PS5Cl and a polar poly(vinylidene fluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) framework is prepared via an electrospinning‐infiltration‐hot‐pressing method. The interaction between Li6PS5Cl and polar P(VDF‐TrFE) ensures a high lithium‐ion conductivity (≈1.2 mS cm–1) at room temperature and good mechanical ductility of the composite electrolyte membrane. The coin‐type ASSB cells with the thin composite electrolyte membrane, a composite cathode of LiNbO3‐coated LiNi0.8Co0.1Mn0.1O2 and Li6PS5Cl, and a lithium‐indium anode, show super cycling performance, and the capacity retention is 92% after 1000 cycles and 71% even after 20 000 cycles at 1.0 mA cm–2 (i.e., 1.61 C) at room temperature. Moreover, pouch‐type ASSB cells with a high mass loading of active materials are made to demonstrate the potential and feasibility in future commercial applications. [ABSTRACT FROM AUTHOR]

ASSLBs, composite solid electrolytes, Li 6PS 5Cl, sulfide electrolytes, P(VDF-TrFE) The flexible composite solid electrolyte membrane enables super long-cycling performance of all-solid-state lithium batteries. Super Long-Cycling All-Solid-State Battery with Thin Li6PS5Cl-Based Electrolyte (Adv. [Extracted from the article]