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Zn metal as one of the promising anodes of aqueous batteries possesses notable advantages, but it faces severe challenges from severe side reactions and notorious dendrite growth. Here, ultrathin nanosheets of α‐zirconium phosphate (ZrP) are explored as an electrolyte additive. The nanosheets not only create a dynamic and reversible interphase on Zn but also promote the Zn2+ transportation in the electrolyte, especially in the outer Helmholtz plane near ZrP. Benefited from the enhanced kinetics and dynamic interphase, the pouch cells of Zn||LiMn2O4 using this electrolyte remarkably improve electrochemical performance under harsh conditions, i.e. Zn powders as the Zn anode, high mass loading, and wide temperatures. The results expand the materials available for this dynamic interphase, provide an insightful understanding of the enhanced charge transfer in the electrolyte, and realize the combination of dynamic interphase and enhanced kinetics for all‐climate performance. [ABSTRACT FROM AUTHOR]

Zn metal as one of promising anode materials for aqueous batteries suffers from notorious dendrite growth, serious Zn corrosion and hydrogen evolution. Here, a bifunctional electrolyte additive, N‐methyl pyrrolidone (NMP), is developed to improve the electrochemical performance of Zn anode. NMP not only alters the solvation structure of Zn2+, but also in situ produces a dense N‐rich solid‐electrolyte‐interphase layer on Zn foils. This layer protects Zn foils from corrosive electrolytes and benefits the uniform plating/stripping of Zn. Hence, the asymmetrical cells with NMP in the electrolyte retain a high coulombic efficiency of 99.8 % over 1000 cycles. The symmetric cells survive ≈200 h for 10 mAh cm−2 at a high Zn utilization of 85.6 %. The full cells of Zn||MnO2 show an impressive cumulative capacity even with lean electrolyte (E/C ratio=10 μL mAh−1), limited Zn supply (N/P ratio=2.3) and high areal capacity (5.0 mAh cm−2). [ABSTRACT FROM AUTHOR]