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Aqueous zinc‐ion batteries (ZIBs) are promising for next‐generation energy storage. However, the reported electrode materials for ZIBs are facing shortcomings including low capacity and unsatisfactory cycling stability etc. Herein, hexaazatrinaphthalene‐quione (HATNQ) is reported for aqueous ZIBs. The HATNQ electrodes delivered an ultrahigh capacity (482.5 mAh g−1 at 0.2 A g−1) and outstanding cyclability of >10 000 cycles at 5 A g−1. The capacity sets a new record for organic cathodes in aqueous ZIBs. The high performances are ascribed to the rich C=O and C=N groups that endowed HATNQ with a 2D layered supramolecular structure by multiple hydrogen bonds in plane with π–π interactions out‐of‐plane, leading to enhanced charge transfer, insolubility, and rapid ion transport for fast‐charge and ‐discharge batteries. Moreover, the 2D supramolecular structure boosted the storage of Zn2+/H+, particularly the storage of Zn2+, due to the more favorable O⋅⋅⋅Zn⋅⋅⋅N coordination in HATNQ. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries (ZIBs) are promising for next‐generation energy storage. However, the reported electrode materials for ZIBs are facing shortcomings including low capacity and unsatisfactory cycling stability etc. Herein, hexaazatrinaphthalene‐quione (HATNQ) is reported for aqueous ZIBs. The HATNQ electrodes delivered an ultrahigh capacity (482.5 mAh g−1 at 0.2 A g−1) and outstanding cyclability of >10 000 cycles at 5 A g−1. The capacity sets a new record for organic cathodes in aqueous ZIBs. The high performances are ascribed to the rich C=O and C=N groups that endowed HATNQ with a 2D layered supramolecular structure by multiple hydrogen bonds in plane with π–π interactions out‐of‐plane, leading to enhanced charge transfer, insolubility, and rapid ion transport for fast‐charge and ‐discharge batteries. Moreover, the 2D supramolecular structure boosted the storage of Zn2+/H+, particularly the storage of Zn2+, due to the more favorable O⋅⋅⋅Zn⋅⋅⋅N coordination in HATNQ. [ABSTRACT FROM AUTHOR]