<p>Urea oxidation reaction (UOR) instead of anodic oxygen evolution reaction (OER) is considered an effective way to reduce energy consumption in electrocatalytic water splitting for hydrogen production. Nevertheless, the slow rate of reaction of UOR, which entails a procedure of transferring six electrons, has hindered its widespread use. Therefore, it is crucial to design highly effective electrocatalysts for the implementation of UOR. Herein, a novel NiCo-hydroxysulfide (NiCo-HOS) electrocatalyst has been reported for UOR, which is obtained by the exchange of sulfur ions in NiCo layered double hydroxide (NiCo-LDH) nanosheets at room temperature. Benefitting from the sulfurization process, the composition, electronic structure, and surface properties of electrocatalysts have undergone significant changes and optimizations. Following sulfurization treatment, the resulting NiCo-HOS showed enhanced chemical resistance to alkaline electrolytes and improved electrical conductivity. In a 40 h operation test, it maintained high stability and provided a stable current density of 100 mA cm⁻² at a relatively low potential of 1.33 V (vs. RHE) in a solution of 1 mol L⁻¹ KOH + 0.5 mol L⁻¹ urea. Subsequently, the anode electrolytic product is analyzed through gas chromatography (GC), and N₂ is detected as the product without the presence of CO, indicating that the urea has undergone complete oxidation.</p>