Transition metal-based oxyhydroxides (MOOH) have garnered significant attention as promising catalyst for the Oxygen Evolution Reaction (OER). However, the direct synthesis of MOOH poses challenges due to the instability of trivalent cobalt and nickel salts, attrivuted to their high oxidation states. In this study, theoretical computations predicted that Co(OH) nanosheets are exclusively formed on carbon structures, owing to the stronger binding energy between CoOOH and CC compared to Co(OH). Furthermore, the presence of FeOOH interface reduces the binding energy between CoOOH and carbon structure. Experiment evidence confirms that CoOOH can be directly synthesized through controlled epitaxial growth on an FeOOH interface using a hydrothermal method. Moreover, the in-situ doping of iron leads to the formation of high-quality FeCoOOH with exceptional OER performance, displaying a low overpotential of 240 mV at 10 mA cm and a small Tafel slope of 43 mV dec. Density functional theory (DFT) calculations uncover the substantial enhancement of oxygen-containing species adsorption abilities by FeCoOOH, resulting in improved OER activity. This work presents a promising strategy for the efficient preparation of layered cobalt oxyhydroxides, enabling efficient energy conversion and storage.