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All‐solid‐state lithium batteries (ASSBs) have the potential to trigger a battery revolution for electric vehicles due to their advantages in safety and energy density. Screening of various possible solid electrolytes for ASSBs has revealed that garnet electrolytes are promising due to their high ionic conductivity and superior (electro)chemical stabilities. However, a major challenge of garnet electrolytes is poor contact with Li‐metal anodes, resulting in an extremely large interfacial impedance and severe Li dendrite propagation. Herein, an innovative surface tension modification method is proposed to create an intimate Li | garnet interface by tuning molten Li with a trace amount of Si3N4 (1 wt%). The resultant Li‐Si‐N melt can not only convert the Li | garnet interface from point‐to‐point contact to consecutive face‐to‐face contact but also homogenize the electric‐field distribution during the Li stripping/depositing process, thereby significantly decreasing its interfacial impedance (1 Ω cm2 at 25 °C) and improving its cycle stability (1000 h at 0.4 mA cm−2) and critical current density (1.8 mA cm−2). Specifically, the all‐solid‐state full cell paired with a LiFePO4 cathode delivered a high capacity of 145 mAh g−1 at 2 C and maintained 97% of the initial capacity after 100 cycles at 1 C. [ABSTRACT FROM AUTHOR]

[Display omitted] • Contact issue of the anode-electrolyte interface was tackled by a Li-Mo composite. • Lower cohesive energy and higher binding energy are beneficial to better contact. • Symmetric cell shows a high critical current density and a stable 1200-h cycling. • A full cell with a LiFePO 4 cathode presented stable performance for 200 cycles. • The work provides a facile and feasible way to overcome interface problems. Interface issues are the biggest challenges that hindering the commercialization of solid-state lithium metal batteries (SSLMBs). Here, we propose a novel strategy targeting for effectively resolving the tedious lithium-garnet solid electrolyte interface problem from the lithium side. We intentionally introduce α-MoO 3 nanobelts into the molten metallic lithium, forming a Li-Mo composite. Compared to molten lithium, the composite improves wettability on the garnet electrolyte. As revealed by density functional theory calculations, such improvement could be ascribed to the reduced cohesive energy and the improved interface binding energy to the LLZTO. Intimate surface contact can be easily achieved without complicated surface treatment, which not only significantly reduces the interface resistance to ~ 1 Ω cm2, but could also effectively inhibits the generation of lithium dendrites. These features ensure a significant critical current density of 1700 µA cm−2 and a stable electrochemical Li plating/stripping process for more than 1200 h. A full cell with the Li-Mo composite anode and LiFePO 4 cathode also presents a fairly stable cycling performance at room temperature. Different from most previous strategies that try to tackle the interface issues from the electrolyte side, our research results suggest that designing lithium composite anodes with low cohesive energy and high interface binding energy to the solid electrolyte is an attractive and feasible solution to overcome interface problems. [ABSTRACT FROM AUTHOR]