Although amorphous materials are popular in oxygen electrocatalysis, their performance requires further improvement to meet the need for rechargeable zinc–air batteries. In this work, an amorphous/crystalline layered manganese oxide (ACMO) was designed, and its unique amorphous/crystalline homogeneous structure activated its oxygen reduction activity with a positive half‐wave potential of 0.81 V and oxygen evolution activity with a moderate overpotential of 407 mV at 10 mA cm−2. Moreover, the amorphous/crystalline structure endowed ACMO with excellent stability. While employed as the air‐electrode material for rechargeable zinc–air batteries, ACMO overcame the poor cycling stability of manganese oxide and cycled stably for 1000 cycles (≈17 days) at 10 mA cm−2. Besides, it delivered a high power density of 159.7 mW cm−2 and a narrow voltage gap of 0.66 V. This work gives an insight into designing oxide materials with amorphous/crystalline structure and feasible guidance for harmonizing electrochemical activity and stability.