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Sodium super ionic conductor (NASICON)‐type Li1.3Al0.3Ti1.7(PO4)3 (LATP) is one of the most promising solid‐state electrolytes (SSEs) owing to its high Li‐ion conductivity, high stability with air, and low cost. However, LATP is less widely deployed due to its high incompatibility with lithium metal. Herein, a facile and inexpensive spray‐coating approach is proposed to construct a thin 3D organic/inorganic...