A novel, rational, and efficient way to explore high-performance electrocatalysts was developed by controlling the reaction kinetics of the rate-determining step (RDS). Density functional theory (DFT) calculations demonstrate that the RDS for the oxygen evolution reaction driven by transition metal hydroxides/oxides, i.e., surface adsorption of (OH-/OOH center dot) species, can be significantly promoted by increasing the electrophilicity of electrocatalysts via hybridization with electron-withdrawing inorganic nanosheets. As predicted by DFT calculation, the hybridization of Ni-Fe-layered double hydroxide (LDH)/Ni-Co-LDH, with RuO2 nanosheets (1.0 wt%) leads to significant lowering of the overpotentials to 207/276 mV at 10 mA cm(-2), i.e., one of the smallest overpotentials for LDH-based materials, with the increase in the current density. The necessity of a very small amount of RuO2 nanosheets (1.0 wt%) to optimize the electrocatalyst activity highlights the remarkably high efficiency of the RuO2 addition. The present study underscores the importance of kinetic control of the RDS via hybridization with electron-withdrawing species for exploring novel efficient electrocatalysts.