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Summary High ionic conductivity at room temperature (RT) and good ion transport capability at electrode/electrolyte interface are fundamental requirements for high‐rate solid‐state lithium batteries (SSBs). In this work, we designed a poly (propylene carbonate) (PPC)‐based organic/inorganic composite solid electrolyte (CSE) membrane with high filling of tantalum‐doped lithium lanthanum zirconium oxide (LLZTO) and functionalized layers for enhancing the RT rate performance of SSB. The synergistic effect of LLZTO and interfacial functionalized layers endows the NCM622/CSE/Li battery with high‐rate and cycling performances at RT. The SSB with 20% LLZTO‐filled solid electrolyte shows the initial capacities of 162.0, 148.5 and 130.1 mAh g−1 at 1C, 2C, and 3C respectively, with retention capacities of 115.6, 104, and 100.6 mAh g−1 after 150 cycles. This strategy for an organic/inorganic CSE is of great practical significance for the development of high‐rate SSBs.

Poor interface stability is a crucial problem hindering the electrochemical performance of solid-state lithium batteries. In this work, a novel approach for interface stability was proposed to integrate the cathode/ solid electrolyte by forming an electrolyte buffer layer on the rough surface of the cathode and coating a layer of graphite on the side of the electrolyte facing the lithium anode. This hybrid structure significantly improves the integration and the interface stability of the electrode/electrolyte. The interfacial resistance was dramatically reduced, the stability of the plating/stripping of Li metal was enhanced, and the growth of lithium dendrites was also inhibited due to the formation of the LiC 6 transition layer. The obtained solid-state lithium battery shows enhanced rate performance at room temperature from 0.5 to 4 C and stable cycling performance at 1 C with a retention capacity of 100 mAh g −1 after 200 cycles. This integrated electrode/electrolyte design approach is expected to be widely used to improve interfacial stability and roomtemperature electrochemical performance of solid-state batteries.