Understanding water splitting in pH-neutral media has important implications for hydrogen production from seawater. Despite their significance, electrochemical water oxidation and reduction in neutral electrolytes still face great challenges. This study focuses on designing efficient electrocatalysts capable of promoting the oxygen evolution reaction (OER) in neutral media by incorporating high-valence elements into transition-metal hydroxides. The as-prepared and optimized two-dimensional Mo-Co(OH)2 nanosheets, which undergo operando transformation into oxyhydroxide active species, demonstrated an overpotential of 550 mV at 10 mA cm-2 with a Tafel slope of 110.1 mV dec-1 in 0.5 M KHCO3. In situ X-ray absorption spectroscopy revealed that the incorporation of high-valence elements facilitates the generation of CoOOH active sites at low potential and enhances electron transfer kinetics by altering the electronic environment of the Co center. This study offers new insights for developing more efficient OER electrocatalysts and provides fresh ideas for seawater utilization through the study of the reaction mechanism of the near-neutral-pH OER.