The application of fuel cells and metal-air batteries is limited by the rate of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Thus, the aim of this study is to find an efficient electrocatalyst to accelerate the reaction rate by DFT method. The structures of VIIB, VIII, IB, and IIB groups transition metals doped g-C9N7 as superb bifunctional electrocatalysts for ORR and OER are probed. The results show that Fe-, Pd-, and Au–C9N7 possess the superb ORR performance with the ORR overpotentials values of 0.35, 0.40, and 0.39 V, which gives them better performance than Pt(111). Moreover, Rh-, Pd-, and Pt–C9N7 have better OER performance with the OER overpotentials values of 0.30, 0.57, and 0.43 V, which makes them comparable to RuO2(110) and IrO2(110). Finally, the calculated bifunctional index (BI) results show that Pd–C9N7 can be used as an excellent bifunctional electrocatalyst because it has a minimum BI value of 0.97 V. This research has the potential to provide valuable theoretical direction into the use of M − C9N7 as electrocatalysts for both the ORR and OER.