ee Zn electrode exhibits high cycling stability and enhanced Coulombic efficiency, which also contributes to enhancement of the full‐cell performance when it is coupled with MnO 2 and LiFePO 4 cathodes.20:T487,Rechargeable aqueous Zn-ion batteries promise high capacity, low cost, high safety, and sustainability for large-scale energy storage. The Zn metal anode, however, suffers from the dendrite growth and side reactions that are mainly due to the absence of an appropriate solid electrolyte interphase (SEI) layer. Herein, the in situ formation of a dense, stable, and highly Zn²⁺ -conductive SEI layer (hopeite) in aqueous Zn chemistry is demonstrated, by introducing Zn(H₂ PO₄ )₂ salt into the electrolyte. The hopeite SEI (≈140 nm thickness) enables uniform and rapid Zn-ion transport kinetics for dendrite-free Zn deposition, and restrains the side reactions via isolating active Zn from the bulk electrolyte. Under practical testing conditions with an ultrathin Zn anode (10 µm), a low negative/positive capacity ratio (≈2.3), and a lean electrolyte (9 µL mAh^-1 ), the Zn/V₂ O₅ full cell retains 94.4% of its original capacity after 500 cycles. This work provides a simple yet practical solution to high-performance aqueous battery technology via building in situ SEI layers.21:T52e,Abstract The corrosion, passivation, and dendritic growth of Zn anodes and the dissolution of cathodes hinder rechargeable aqueous zinc ion battery (AZIB) rejuvenation. In this work, a versatile Zn‐based montmorillonite (MMT) interlayer is constructed to achieve a stable rechargeable AZIB. The Zn‐based MMT coating Zn foil (MMT‐Zn) is designed to enable a high transference number for Zn 2+ ( t + ≈ 0.82) and a freeway for Zn 2+ migration to alleviate corrosion and passivation and suppress Zn dendrites. The results show the MMT‐Zn symmetrical batteries render dendrite‐free plating/stripping with an ultra‐stable and small overpotential (50 mV) and a long‐life span (1000 cycles) at 1 mA cm −2 /0.25 mAh cm −2 and with 100 mV overpotential at ultrahigh current and capacity of 10 mA cm −2 /45 mAh cm −2 (over 1000 h, 77% depth of discharge). The MMT interlayer is applied to the MnO 2 cathode to inhibit the discharge product dissolving and diffusing into the electrolyte, so that the stability of the capacity is maintained. Thus, MMT‐Zn||MMT‐MnO 2 delivers an ultra‐long cycle life and ultra‐high capacity (1100 cycles with 191.5 mAh g −1 at 2 C). Hopefully, Zn‐based MMT interlayer can be considered to improve the electrochemical performance of the metal anodes and soluble cathodes.22:T581,

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