Metal–organic frameworks (MOFs) have recently garnered immense attention for their applications in the oxygen evolution reaction (OER) during electrochemical water splitting, owing to their exceptional characteristics such as high specific surface area (SSA), abundant and regular porosity, and flexibility in their framework, dimension, geometry, and functionality of metal active sites. It is speculated that the incorporation of additional transition metals into the MOF network effectively enhances the material’s electrocatalytic activities. In this study, we synthesized a bimetallic CoFeBTC MOF with an SSA of 310.59 m2g–1 using a simple, inexpensive one-step solvothermal approach and employed it for OER applications. The CoFeBTC MOF demonstrated superior electrocatalytic activity, achieving an overpotential of 310 mV at 10 mA cm–2 and a Tafel slope of 122 mV dec–1 in an alkaline medium (1 M KOH) electrolyte. Notably, the synergistic interaction between cobalt (Co) and iron (Fe) in the bimetallic framework significantly boosts the electrochemical activity toward the OER compared to individual CoBTC and FeBTC MOFs. This solvothermal technology and its synergistic effect may encourage researchers to explore and develop more reliable and efficient electrocatalysts for energy conversion.