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Aqueous polysulfide/iodide redox flow batteries are attractive for scalable energy storage due to their high energy density and low cost. However, their energy efficiency and power density are usually limited by poor electrochemical kinetics of the redox reactions of polysulfide/iodide ions on graphite electrodes, which has become the main obstacle for their practical applications. Here, CoS2/CoS heterojunction nanoparticles with uneven charge distribution, which are synthesized in situ on graphite felt by a one-step solvothermal process, can significantly boost electrocatalytic activities of I−/I3− and S2−/Sx2− redox reactions by improving absorptivity of charged ions and promoting charge transfer. The polysulfide/iodide flow battery with the graphene felt-CoS2/CoS heterojunction can deliver a high energy efficiency of 84.5% at a current density of 10 mA cm−2, a power density of 86.2 mW cm−2 and a stable energy efficiency retention of 96% after approximately 1000 h of continuous operation. Polysulfide/iodide redox flow batteries are promising due to low cost and high-solubility components, but are limited by energy efficiency and power density. Here the authors fabricate heterojunction electrocatalysts to achieve improved performance in a polysulfide/iodide redox flow battery. [ABSTRACT FROM AUTHOR]