To achieve a sustainable and clean future, water electrolysis is of great importance to produce hydrogen and oxygen. Also, due to the sluggish process of reaction, it is crucial to fabricate high-performance oxygen evolution reaction (OER) catalysts to increase the overall efficiency of water electrolysis. In this study, we present a remarkably thin Co−Fe phosphide/carbon (CFP) nanosheet for the OER catalyst. The fabrication of CFP nanosheet is accomplished by three easy steps, which start with the synthesis of Co-and Fe-based brucite-type metal hydroxide (CFT) using an organic linker. Then, CFT undergoes subsequent oxidation and phosphorization to become CFP. During post-treatment, the organic linker becomes a carbon composite and remains on the CFP nanosheet which could benefit the overall catalytic efficiency. CFP nanosheet is equipped with a thickness of 7.67 nm on average, which is recognizably low considering the post-treatments. The electrochemical OER performance of CFP nanosheet implies high catalysis capability toward OER with the overpotential of 277 and 362 mV to reach the current density of 10 and 150 mA•cm −2 , respectively. To investigate the catalytic active site, ex situ XPS analysis shows some beneficial characteristics of CFP nanosheet that benefit the OER catalysis overall. The investigation suggests that reactive oxyhydroxides (peroxo-like O 2 2− species) are formed via surface reconstruction and gradually increase during the OER catalysis. This phenomenon implies the synergistic effect between Co and Fe, which is determined by electrochemical measurements. Also, the evidence of lattice oxygen implies the possible OER mechanism in which the involvement of the oxygen intermediates is crucial. The utilization of our investigation can be extended to other fields of energy material synthesis, which include batteries, supercapacitors, and even other electrochemical catalysts.