LAUSR

The high Zn ion desolvation energy, sluggish Zn deposition kinetics, and top Zn plating pattern are the key challenges toward practical Zn anodes. Herein, these key issues are addressed by introducing zinc pyrovanadate (ZVO) as a solid zinc‐ion conductor interface to induce smooth and fast Zn deposition underneath the layer. Electrochemical studies, computational analysis, and in situ observations reveal the boosted desolvation and deposition kinetics, and uniformity by ZVO interface. In addition, the anti‐corrosion ability of Zn anodes is improved, resulting in high Zn stripping/plating reversibility. Consequently, the ZVO layer renders fast rechargeability and durable life in both Zn symmetric cells (1050 h at 10 mA cm−2, 1 mAh cm−2) and Zn/V2O5 batteries (79.1% capacity retention after 1000 cycles at 2 A g−1) with low electrode polarization. This work provides insights into the design of solid zinc‐ion conductor interface to enhance the interface stability and kinetics of Zn metal anodes.