| Summary: | The performance of solid‐state Li‐metal batteries (SSLBs) with argyrodite solid electrolytes (SEs) is limited by interfacial side reactions at the Li‐metal/SE interface. In this study, we introduce Li3N interfacial layer as a stabilizer at the Li/SE interface based on its good electrochemical and mechanical properties. The Li3N is synthesized onto the Li‐metal substrate in micrometer thickness through a straightforward treatment of Li‐metal in a N2‐filled glovebox, as confirmed by plasma focused ion beam analysis. The Li3N interfacial layer exhibits outstanding cycling stability in its symmetrical cell for over 5000 cycles, equivalent to 6000 h of operation, while the bare Li symmetrical cell endures only 257 cycles. Multimodal characterization techniques coherently demonstrate that the Li3N interfacial layer contributes to reducing mechanical resistance (e.g., voids, microcracks) at the Li/SE interface, as well as charge–transfer resistance during cycling in full‐cells, particularly when paired with LiNbO3‐coated LiNi0.6Mn0.2Co0.2O2 (NMC622) cathode. Furthermore, the Li3N interfacial layer not only enhance specific capacity (178 mAh g−1) and Coulombic efficiency (>99% at the 2nd cycle) but also improve the rate capability of the SSLB full cells. Our study highlights the promising strategy of employing Li3N as an interfacial layer for stabilizing the Li/SE interface in SSLBs.
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