Because of the adjustable electronic structure of bimetallic alloys, they have received much attention in electrocatalytic reactions. However, to date, there is a lack of effective methods to synthesize bimetallic nanoalloys with controllable metal proportions in the active species of the catalysts prepared by a high-temperature annealing method, leading to inferior catalytic activity and difficulty in identifying the active sites. Here, we synthesize iron (Fe)−cobalt (Co)-based nanoparticles coated with a few layers of amorphous carbon shell (<1 nm) and with Co 7 Fe 3 alloy as the core by facile pyrolysis of a bimetallic Fe−Cobased tartrate, which exhibits excellent oxygen evolution reaction (OER) activity with a low overpotential of 272 mV at a current density of 10 mA cm −2 and good durability in alkaline media. Compared with single-metal Fe/Co tartrate-derived catalysts, a bimetallic Fe−Co tartrate-derived catalyst with Co 7 Fe 3 O x active sites shows higher charge-transfer ability and a lower OER barrier (approximately 285 kJ mol −1 ). For the first time, this work demonstrates that Fe−Co-based tartrate complexes can be used as precursors to construct high-performance bimetallic Fe−Co-based nanocomposite catalysts with controllable active sites for electrocatalytic OER.