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Abstract In this work, the Na–K liquid alloy with a charge selective interfacial layer is developed to achieve an impressively long cycling life with small overpotential on a sodium super‐ionic conductor solid‐state electrolyte (NASICON SSE). With this unique multi‐cation system as the platform, we further propose a unique model that contains a chemical decomposition domain and a kinetic decomposition domain for the interfacial stability model. Based on this model, two charge selection mechanisms are proposed with dynamic chemical kinetic equilibrium and electrochemical kinetics as the manners of control, respectively, and both are validated by the electrochemical measurements with microscopic and spectroscopic characterizations. This study provides an effective design for high‐energy‐density solid‐state battery with alkali Na–K anode, but also presents a novel approach to understand the interfacial chemical processes that could inspire and guide future designs.