Due to its high theoretical energy density, good safety, and availability, as well as low cost, the rechargeable aqueous zinc-ion battery is considered one of the most promising systems for the next generation of energy storage devices. However, due to the strong electrostatic interaction between Zn 2+ and host and the proton/Zn 2+ cointercalation in aqueous media, the development of a zinc-ion battery with high capacity and a long lifetime remains an uphill task. In this work, a novel electrode−electrolyte design is employed by using a ZIF/ Zn heterostructure as a microporous host matrix and an organic zinc trifluoromethanesulfonate as the constituent of the electrolyte. A zincion battery based on the ZIF/Zn heterostructure anode delivers a specific capacity of 149 mAh g −1 and maintains a retention as high as 80% after 330 cycles at 1 A g −1 . The synergistic effect of microstructural ZIF and hydrophobic trifluoromethanesulfonate anions creates a unique electrode−electrolyte interface, which suppresses the formation of dendrites and self-discharge of the Zn anode, resulting in the long cycling stability of the aqueous zinc-ion batteries.

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