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High‐voltage manganese‐based materials are considered as promising cathode materials for aqueous zinc‐ion batteries (AZIBs). Herein, oxygen vacancy‐rich K0.5Mn2O4 sheets were anchored uniformly onto honeycomb‐like interconnected carbon nanoflakes (CNF@K0.5Mn2O4) for AZIB cathode applications. In the composite, the CNFs provided excellent intergranular electron transport capability, while the oxygen vacancies enhanced the electron transport efficiency inside crystals, and the embedded K ions expanded the interlayer spacing and stabilized the layered crystal structure. A reversible specific capacity of 241 mAh g−1 could be maintained by the composite at 0.5 A g−1 for 400 cycles. A combination of ex‐situ analytical methods and density functional theory calculations was carried out to elucidate the electrochemical mechanism of reversible zinc storage. In addition, flexible quasi‐solid‐state batteries of Zn//CNF@K0.5Mn2O4 were constructed by substituting the traditional aqueous electrolyte for a quasi‐solid‐state gel electrolyte, which worked efficiently and exhibited high bending durability.

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