Developing zinc-air batteries still heavily relies on the design of stable, high-activity, and inexpensive oxygen-electric bifunctional catalysts. In this work, transition metal iron salts converted amorphous carbon into graphitized carbon at high temperatures, and nitrogen-doped graphitized carbon-anchored iron nanoparticles (Fe–N–C) are prepared. Then, Fe–N–C is pyrolyzed with selenium dioxide (SeO2) to convert iron (Fe) nanoparticles into iron selenide (FeSe) in situ to obtain nitrogen-doped graphitized carbon-anchored FeSe nanoparticle catalysts (FeSe/NC). The catalyst's carbon support has excellent electrical conductivity, which effectively promotes the transport rate of charges and enhances the catalytic activity of FeSe particles. FeSe/NC demonstrates outstanding catalytic activity for both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). When utilizing FeSe/NC catalysts in rechargeable zinc-air batteries (ZABs-FeSe/NC), the most excellent power density could exceed 186.6 mW cm−2, and the specific capacity can achieve 905.2 mAh g−1, demonstrating excellent performance. Furthermore, the battery can achieve stable charge-discharge for longer than 200 h at a large current density of 10 mA cm−2, which has excellent practical application feasibility in the future.