Exploring efficient and stable oxygen evolution reaction (OER) catalysts with earth-abundant elements has been an urgent task in water splitting. Metal–organic frameworks (MOFs), possessing abundant active metal sites and tunable porous crystalline structures, are promising as OER catalysts. In this paper, a MOF based on benzotriazole-5-carboxylate (Co₃-btca) that contains unsaturated coordinated metal centers and a 1D channel was selected to act as an OER catalyst. To optimize the OER performance, isostructural bimetallic and trimetallic frameworks were obtained by doping with Fe and/or Ni ions. The optimized Co_2.36Fe_0.19Ni_0.45-btca possesses the lowest overpotential of 292 mV at 10 mA cm⁻² and a small Tafel slope of 72.6 mV dec⁻¹. The enhanced catalytic performance could be attributed to the synergistic effect between the unsaturated coordinated Co, Fe and Ni sites, which are beneficial for the nucleophilic attack of OH⁻ forming adsorption intermediates.