The urgent need to alleviate global warming and limit the consumption of fossil fuels has prompted the development of rechargeable Zn-air batteries (ZABs) considering their superior energy density, safety, and cost-effectiveness. However, the sluggish reaction kinetics of the oxygen evolution reaction (OER) and the unfavorable properties of conventional OER catalysts (including low electrical conductivity and the use of active site-blocking binders) hinder the development of practically viable ZABs. Herein, we report a distinct approach for directly synthesizing cobalt-doped nickel oxide (Co-NiO) with a chiral structure on porous Ni foam via a one-step hydrothermal process. The chirality-induced spin selectivity (CISS) boosts the OER kinetics, while Co doping elevates the electrical conductivity and the abundance of active sites on the catalyst. The chiral Co-NiO demonstrates an OER current density of 10 mA cm<sup>-2</sup> at 1.58 V versus the reversible hydrogen electrode, outperforming both achiral Co-NiO and undoped NiO. Furthermore, a chiral Co-NiO-based rechargeable ZAB demonstrates a high open-circuit potential (1.57 V), a low charge/discharge overpotential (0.71 V), and excellent stability for 960 h (40 days) because the CISS effect mitigates the production of the corrosive singlet oxygen. These results represent a prominent pathway for the advancement of ZABs using the low-cost oxygen evolution catalyst modulated by the CISS effect and heteroatomic doping.