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Carbon nanomaterials doped with N and B could activate nearby carbon atoms to promote charge polarization through the synergistic coupling effect between N and B atoms, thus facilitating adsorption of O 2 and weakening O-O bond to enhance oxygen reduction reaction. Herein, a simple and controllable self-assembly strategy is applied to synthesize porous B, N co-doped carbon-based catalysts (BCN-P), which employs the macrocyclic molecule cucurbit[7]uril (CB7) as nitrogen source, and 3D aromatic-like closo-[B 12 H 12 ] 2- as boron source. In addition, polystyrene microspheres are added to help introduce porous structure to expose more active sites. Benefitting from porous structures and the synergistic coupling effect between N and B atoms, BCN-P has a high onset potential (E onset =0.846 V) and half-wave potential (E 1/2 =0.74 V) in alkaline media. The zinc-air battery assembled with BCN-P shows high operating voltage (1.42 V), peak power density (128.7 mW cm -2 ) and stable charge/discharge cycles, which is even comparable with Pt/C., (© 2024 Wiley-VCH GmbH.)