Aqueous zinc batteries (AZBs) feature high safety and low cost, but intricate anodic side reactions and dendrite growth severely restrict their commercialization. Herein, ethylenediaminetetraacetic acid (EDTA) grafted metal-organic framework (MOF-E) is proposed as a dually-functional anodic interphase for sustainable Zn anode. Specifically, the target-distributed EDTA serves as ion-trapped tentacles to accelerate the desolvation and ionic transport by powerful chemical coordination, while the MOF offers suitable ionic channels to induce oriented deposition. As a result, MOF-E interphase fundamentally suppresses side reactions and guides horizontally arranged Zn deposition with (002) preferred orientations. The Zn|MOF-E@Cu cell exhibits a markedly improved Coulombic efficiency of 99.7% over 2500 cycles, and the MOF-E@Zn|KVOH (KV12O30-y·nH2O) cell yields a steady circulation of 5000 cycles@90.47% at 8 A g-1.