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The corrosion, parasitic reactions, and aggravated dendrite growth severely restrict development of aqueous Zn metal batteries. Here, we report a novel strategy to break the hydrogen bond network between water molecules and construct the Zn(TFSI)2‐sulfolane‐H2O deep eutectic solvents. This strategy cuts off the transfer of protons/hydroxides and inhibits the activity of H2O, as reflected in a much lower freezing point (<−80 °C), a significantly larger electrochemical stable window (>3 V), and suppressed evaporative water from electrolytes. Stable Zn plating/stripping for over 9600 h was obtained. Based on experimental characterizations and theoretical simulations, it has been proved that sulfolane can effectively regulate solvation shell and simultaneously build the multifunctional Zn‐electrolyte interface. Moreover, the multi‐layer homemade modular cell and 1.32 Ah pouch cell further confirm its prospect for practical application. [ABSTRACT FROM AUTHOR]

[Display omitted] • A bifunctional strategy is proposed to enhance Zn (0 0 2) plane over prolonged cycling. • Carboxylated chitosan (CCS) is demonstrated as a bifunctional electrolyte additive. • CCS can selectively etch Zn matrix with (0 0 2) texturing. • CCS can induce the assembly of Zn atoms along (0 0 2) direction. • Zn anodes with CCS exhibit extended cycling stability and high utilization rate. Although Zn (0 0 2) crystal plane make it highly competitive for the design of high-performance Zn anodes, manipulating the Zn (0 0 2) crystal plane and maintaining long-term stability are significant challenges. Herein, carboxylated chitosan (CCS) is introduced as a novel bifunctional polymer electrolyte additive to protect the intrinsic Zn (0 0 2) plane from resolution and induce the highly oriented assembly of Zn atoms along (0 0 2) direction, thereby self-adaptively enhancing the Zn (0 0 2) plane over prolonged cycling. Specifically, CCS with electron-rich groups can preferentially adsorb on Zn anode, selectively etch the Zn anode with (0 0 2) texturing and appropriately affect the assembly of Zn atoms along the (0 0 2) direction. As a result, a remarkable cycling lifespan of over 300 h is achieved at 30 mA cm−2 under a deep depth of discharge of 60 %. Moreover, a highly reversible Zn anode with a high Coulombic efficiency of 99.8 % can also be achieved at 10 mA cm−2 over 1000 cycles. Furthermore, the capacity stability of NH 4 V 4 O 10 ||Zn full cell and Zn||AC hybrid supercapacitor is significantly improved even under harsh conditions, such as high areal capacity, limited Zn resource and lean electrolyte. The CCS additive maintains a stable effect on the directional reconstruction of Zn anodes over prolonged cycling. [ABSTRACT FROM AUTHOR]