Abstract Utilizing affordable bifunctional catalysts per strong ORR/OER (oxygen reduction and evolution reactions) ability and superior zinc‐air battery performance is yet difficult due to the diverse mechanisms of ORR/OER. This work uses CoNi‐MOF (metal‐organic framework) as a self‐template to yield the CrS doped CoNi/C bifunctional catalyst. Comparable to Pt/C and IrO 2 commercial catalysts, the CrS@CoNi/C catalyst exhibits improved electrocatalytic activity toward OER and ORR due to its linked pellet architecture and intact metal sulfide@carbon structure. The CrS@CoNi/C catalyst has the most intriguing ORR/OER performance, with a significantly lower potential and an exceptionally extended cycle duration (E 1/2 = 0.72 V and η 10 = 260 mV). The CrS@CoNi/C‐based aqueous zinc‐air battery shows long‐term charge–discharge stability (more than 100h/600 cycles) together with significant specific capacity (789.7 mAh g −1 Zn ) and power density (132.2 mW cm −2 ). Most significantly, after charge–discharge stability, the recharged CrS@CoNi/C‐based alkaline zinc‐air battery has been employed to exhibit less structural deformation for the cathode and more zincate ion production for the anode side electrodes, which is employed through TEM analysis.