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The Zn-air battery is a promising next-generation battery because of the higher energy density and safety compared with the Li-ion battery. However, the Zn-air battery suffers from huge energy loss and poor cycling performance, which are due to the sluggish kinetics of oxygen reduction/evolution reactions (ORR/OER) and the instability of bifunctional catalysts. The state-of-the-art bifunctional catalyst is the composite of Pt and Ir/Ru oxides, which is hindered by the scarce resource and high cost. Therefore, developing low-cost and high-efficient bifunctional non-noble metal-based catalysts is essential to the deployment of Zn-air batteries. Herein, we report a dual-nitrogen-source mediated pyrolysis route to rationally design and synthesize the hybrid Co/Co–N–C bifunctional catalyst. The tailored catalyst consisting of carbon confined Co nanoparticles and atomically dispersed Co–N–C moiety is identified. Remarkably, the dual-nitrogen-source derived Co/Co–N–C catalyst demonstrates excellent electrochemical performances with a half-wave potential of 0.882 V for ORR and a potential of 1.640 V at 10 mA cm−2 for OER; reasonably, the bifunctionality of Co/Co–N–C, which is supported by the excellent self-breathing Zn-air battery performance (the maximum energy density of 897.1 Wh kg Zn −1; no obvious degradation within 167h cycling). The abundant Co-Nx sites and metallic Co nanoparticles synergistically boost the ORR and OER. Image 1 • A dual-nitrogen-source method is proposed to synthesize porous Co-based catalysts. • The dual nitrogen sources play different roles in morphology and structure control. • The hybrid carbon-confined Co nanoparticles and Co-N x sites are well tailored. • The good bifunctionality is due to the hybrid active site configuration. • Excellent performance and lifetime are obtained in a Zn-air battery. [ABSTRACT FROM AUTHOR]