Various cathode materials have been proposed for high‐performance rechargeable batteries. Vanadyl phosphate is an important member of the polyanion cathode family. VOPO4 has seven known crystal polymorphs with tunneled or layered frameworks, which allow facile cation (de)intercalations. Two‐electron transfer per formula unit can be realized by using VV/VIV and VIV/VIII redox couples. The electrochemical performance is closely related to the structures of VOPO4 and the types of inserted cations. This Review outlines the crystal structures of VOPO4 polymorphs and their lithiated phases. The research progress of vanadyl phosphate cathode materials for different energy storage systems, including lithium‐ion batteries, sodium‐ion batteries, potassium‐ion batteries, multivalent batteries, and supercapacitors, as well as the related mechanism investigations are summarized. It is hoped that this Review will help with future directions of using vanadyl phosphate materials for energy storage.

An amphoteric compound of betaine is demonstrated as an electrolyte additive for aqueous zinc batteries. It forms hydrogen bonds with water and preferentially adsorbs on the Zn surface, which inhibits side reactions and ensures uniform Zn deposition.

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The decomposition of the VOPO4·2H2O cathode material in aqueous zinc batteries is inhibited by a hydrogen bond regulator to suppress water activity.

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The back-deposition of dissolved Mn2+ is a key factor for stable cycling of MnO2 cathodes in aqueous zinc batteries.

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