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Aqueous redox flow batteries (ARFBs) have received considerable attention for large-scale energy storage because of their salient feature of decoupled energy storage and power generation; however, their deployment is critically constrained by low energy density and relatively high cost. Here, we report a low-cost, high-capacity ferrocyanide/ferricyanide ([Fe(CN)₆]^4−/3−)-based electrolyte system via the redox targeting reactions with Prussian blue (Fe₄[Fe(CN)₆]₃, PB). The [Fe(CN)₆]^4−/3−-PB electrolyte exhibits an excellent capacity retention of 99.991% per cycle and an unprecedented capacity of 61.6 Ah L⁻¹. A Zn/[Fe(CN)₆]³⁻-PB flow cell with energy density of 97.4 Wh L⁻¹ at 20 mA cm⁻² and a [Fe(CN)₆]^4−/3−/Br⁻ flow cell with PB as the sole solid material were demonstrated. The battery chemistry and associated redox targeting reactions were scrutinized with computational, neutron diffraction, and …