Bifunctional oxygen catalyst is an important component in the cathode for rechargeable zinc‐air batteries. MnO2 catalysts have aroused intense interests owing to their promising activity for oxygen reduction reaction (ORR), which, however, is still not comparable to precious metal catalysts. To improve the ORR catalysis and meet the requirement for a bifunctional oxygen catalyst, MnO2 nanosheets are modified with Co, Ni or Fe via a facile solution‐based method. Among the modified samples, Co−MnO2 presents improved catalysis for both ORR and oxygen evolution reaction (OER). The modification introduces additional active sites for OER and induced more oxygen defects to further facilitate the ORR. Zn‐air batteries with the Co−MnO2 air cathode showed a higher peak power density of 167 mW cm−2, a lower potential gap of 0.75 V and a higher round‐trip efficiency of 63 % (5 mA cm−2) compared to MnO2 without modification. Good cycling stability of the battery is also achieved. The proper amount of cobalt species in the MnO2 is vital for achieving a balance between high performance and durable cycling.