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Abstract Developing high performance nonprecious metal‐based electrocatalysts has become a critical first step towards commercial applications of metal‐air batteries. Herein, nanocomposites based on Co/Co₂P nanoparticles encapsulated within hierarchically porous N, P, S co‐doped carbon are prepared by controlled pyrolysis of zeolitic imidazolate frameworks (ZIF‐67) and poly(cyclotriphosphazene‐co‐4,4’‐sulfonyldiphenol) (PZS). The resulting Co/Co₂P@NPSC nanocomposites exhibit apparent oxygen reduction reaction (ORR) and evolution reaction (OER) catalytic performance, and are used as the reversible oxygen catalyst for zinc‐air batteries (ZABs). Density functional theory (DFT) calculations exhibit that Co₂P could provide active sites for the ORR and promote the conversion between the adsorbed intermediates, and porous N,P,S co‐doped carbon with Co₂P nanoparticles also improves the exposure of actives sites and endows charge transport. Liquid‐state ZABs with Co/Co₂P@NPSC as the cathode catalysts demonstrate the greater power density of 198.1 mW cm⁻²and a long cycling life of 50 h at 10 mA cm⁻², likely due to the encapsulation of Co/Co₂P nanoparticles by the carbon shell. Solid‐state ZABs also display a remarkable performance with a high peak power density of 74.3 mW cm⁻². Therefore, this study indicates the meaning of the design and engineering of hierarchical porous carbon nanomaterial as electrocatalyst for rechargeable metal‐air batteries.