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Aqueous zinc-ion batteries (AZIBs) are one of the promising energy storage systems, which consist of electrode materials, electrolyte, and separator. The first two have been significantly received ample development, while the prominent role of the separators in manipulating the stability of the electrode has not attracted sufficient attention. In this work, a separator (UiO-66-GF) modified by Zr-based metal organic framework for robust AZIBs is proposed. UiO-66-GF effectively enhances the transport ability of charge carriers and demonstrates preferential orientation of (002) crystal plane, which is favorable for corrosion resistance and dendrite-free zinc deposition. Consequently, Zn|UiO-66-GF-2.2|Zn cells exhibit highly reversible plating/stripping behavior with long cycle life over 1650 h at 2.0 mA cm−2, and Zn|UiO-66-GF-2.2|MnO2 cells show excellent long-term stability with capacity retention of 85% after 1000 cycles. The reasonable design and application of multifunctional metal organic frameworks modified separators provide useful guidance for constructing durable AZIBs.

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Aqueous zinc‐ion batteries feature high safety, low cost, and relatively high energy density; however, their cycle life is hindered by severe Zn dendrite formation and water‐induced parasitic reactions. Herein, a porous polyaniline (PANI) interfacial layer is developed on the surface of Zn metal anode to regulate the transport and deposition of Zn2+, achieving an ultra‐stable and highly reversible Zn anode. Specifically, the abundant polar groups (NH and N) in PANI have a strong attraction to H2O, which can trap and immobilize H2O molecules around Zn2+. Moreover, the protective layer regulates ion flux and deposition behavior of Zn2+ through the ion confinement effect. Consequently, the Zn@PANI anode exhibits improved reversible plating/stripping behavior with a low nucleation overpotential (37.9 mV) at 2.0 mA cm‐2 compared to that of bare Zn anode. The MnO2//Zn@PANI cell demonstrates a high capacity retention of 94.3% after 1000 cycles at 1.0 A g−1. This study lays the foundation for accessible interface engineering and in‐depth mechanistic analysis of Zn anode.