Aqueous Zn-ion energy-storage deviceswith metal Zn as anodes, including batteries and capacitors (ZIBs and ZICs), is largely hindered by dendritic growth and low coulombic efficiency since the side reactions between Zn anodes and electrolyte, originating fromthat targeted and efficient isolation of H 2 O and SO 4 2− is extremely challenging. Herein, inspired by density functional theory (DFT) that the 2D angstrom level metal-organic framework(2D-MOF) is highly selective for the passage of ions, simultaneously excluding the SO 4 2− and H2O but allowing Zn 2 + selective conduction. Moreover, 2D-MOF exhibits better mechanical strength compared with 3D-MOF, which is more conducive to inhibit dendrite growth. Impressively, benefiting from the 2D-MOFlayer, symmetric Zn cells survived up to 2000 h at 4 mA cm −2 ,near 20-times that of bare Zn anodes. Coupling it with cathode for ZICs and ZIBs, excellent electrochemical performances are presented. Importantly, symmetric Na cells with 2D-MOF as ionic sieve membrane also deliver small polarization and outstanding performance, indicating that this study provides an efficient strategy to develop long-life metal anode.