We have achieved the synthesis of dual-metal single atoms and atomic clusters that co-anchor on a highly graphitic carbon support. The catalyst comprises Ni 4 (and Fe 4 ) nanoclusters located adjacent to the corresponding NiN 4 (and FeN 4 ) single-atom sites, which is verified by systematic X-ray absorption characterization and density functional theory calculations. A distinct cooperation between Fe 4 (Ni 4 ) nanoclusters and the corresponding FeN 4 (NiN 4 ) atomic sites optimizes the adsorption energy of reaction intermediates and reduces the energy barrier of the potential-determining steps. This catalyst exhibits enhanced oxygen reduction and evolution activity and long-cycle stability compared to counterparts without nanoclusters and commercial Pt/C. The fabricated Zn−air batteries deliver a high power density and long-term cyclability, demonstrating their prospects in energy storage device applications.