Abstract: Developing low-cost yet efficient oxygen reduction reaction (ORR) electrocatalysts is of paramount importance for the widespread application of renewable energy technologies. Here, a promising catalyst of the Co–Ni nanoalloy–organic framework (Co–Ni NOF) that significantly accelerates the ORR kinetics process has been synthesized by a straightforward pyrolysis strategy. This Co–Ni NOF catalyst with robust stability and strong methanol tolerance exhibits remarkable ORR activity with an excellent half-wave potential of 0.88 V (30 mV superior to that of commercial Pt/C) and an outstanding kinetic current density of 162.9 mA/cm2 at 0.80 V in 0.1 M KOH, which is 17 times that of Pt/C and outperforms most non-noble catalysts reported so far. The electronic structure characterizations d