It is urgent to design a low‐cost electrocatalyst with high activity to enhance the efficiency of oxygen evolution reaction (OER), which is limited by the slow four‐electron transfer kinetics process. Nevertheless, traditional synthetic methods, including calcination and solvothermal, of the electrocatalysts are high‐cost, low‐yield, and energy‐hogging, which limits their industrial application. Herein, an ambient fast synthetic method is developed to prepare terrace‐like Fe/Co bimetal‐organic framework (TFC‐MOF) electrocatalyst materials in gram scale in 1 h. The method in this paper is designable based on coordination chemistry. Fe and Co ions can coordinate with the carboxyl groups on benzene‐1,3,5‐tricarboxylic acid (H3BTC) to form a 2D‐MOF structure. Structural characterizations, including SEM, TEM, and XRD are conducted to verify that the TFC‐MOF is a terrace‐like layered structure with uniform‐sized mesoporous, which reduces the adsorption steric hindrance and facilitates the mass and electron transfer efficiency of OER. The TFC‐MOF shows low overpotential, 255 mV at a current density of 10 mA cm−2, and a low Tafel slope of 49.9 mV dec−1, in an alkaline solution. This work provides a planar coordination strategy to synthesize 2D‐MOF OER electrocatalyst on a large scale with low cost and low energy consumption, which will promote its practical OER applications.