| Summary: | Li<sub>6.3</sub>La<sub>3</sub>Zr<sub>1.65</sub>W<sub>0.35</sub>O<sub>12</sub> (LLZO)-Li<sub>6</sub>PS<sub>5</sub>Cl (LPSC) composite electrolytes and all-solid-state cells containing LLZO-LPSC were fabricated by cold pressing at room temperature. The LPSC:LLZO ratio was varied, and the microstructure, ionic conductivity, and electrochemical performance of the corresponding composite electrolytes were investigated; the ionic conductivity of the composite electrolytes was three or four orders of magnitude higher than that of LLZO. The high conductivity of the composite electrolytes was attributed to the enhanced relative density and the rule of mixture for soft LPSC particles with high lithium-ion conductivity (~10<sup>−4</sup> S·cm<sup>−1</sup>). The specific capacities of all-solid-state cells (ASSCs) consisting of a LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) cathode and the composite electrolytes of LLZO:LPSC = 7:3 and 6:4 were 163 and 167 mAh·g<sup>−1</sup>, respectively, at 0.1 C and room temperature. Moreover, the charge–discharge curves of the ASSCs with the composite electrolytes revealed that a good interfacial contact was successfully formed between the NCM811 cathode and the LLZO-LPSC composite electrolyte.
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