Metal‐organic frameworks (MOFs) have been widely studied as electrocatalysts, and the research strategy to improve their electrocatalytic oxygen evolution reaction (OER) performance is to modify their structure. In this paper, two‐dimensional bimetallic MOFs were constructed to improve electrocatalytic OER performance. Using a mild electrochemical method with Ni and Co as metal sources and 4, 4 ′‐biphenyl dicarboxylic acid (H2BPDC) as ligand, two‐dimensional NiCo‐BPDC was synthesized and then deposited on a carbon cloth electrode. The results show that NiCo‐BPDC/CC possessed a low overpotential of 356 mV at a current density of 20 mA cm−2 with a small Tafel slope of 86 mV dec−1 in 1.0 M KOH solution. The two‐dimensional NiCo‐BPDC exhibits excellent electrocatalytic OER performance because the coordination of Ni and Co in the material and the interaction of the two‐dimensional materials provide a large electrochemically active surface area and expose more metal active sites for OER, thus improving the reaction efficiency and indicating NiCo‐BPDC as potential OER electrocatalyst. Key electrochemical synthesis: A key electrochemical synthesis method was employed to synthesize 2D NiCo‐BPDC MOFs material, which demonstrated simplicity, speed, and efficiency. This material was further utilized for electrocatalytic OER, showcasing the high‐efficiency oxygen evolution capability of its ultra‐thin nanosheet structure under electric action.