Aiming to explore novel oxygen reduction reaction (ORR) catalysts with advanced electrochemical performance and economical and long-term stability is crucial to fuel cells or metal-air batteries. Herein, ordered Pt-Fe intermetallic with an ultralow Pt loading is facilely achieved via the thermal treatment of Pt nanocrystals anchored to the Fe, N-codoped surface-functioned carbon derived from zeolitic imidazolate frameworks. Benefiting from the ordered Pt-Fe intermetallic formed by the rationally applied calcination treatment, the optimized catalyst shows a larger mass activity and better long-term durability compared with Pt/C. Besides, when the optimized sample is applied in the configuration of a zinc-air battery system, it has a higher maximum power density, a better specific capacity as well as a longer discharge time, surpassing those of the Pt/C catalyst.