In this work, we are enhancing the catalytic activity of the urea electrooxidation (UEO) process by using the composite of polyaniline (Pani), nickel oxide (NiO), and polymorphs of manganese oxide (MnOx) based on a graphite electrode. The hydro‐gel method was used to prepare catalyst suspension with different ratios from NiO and MnOx. The chemical structures and surface morphology were characterized by employing the IR, XRD, and SEM/EDEX techniques. The catalytic activity of four modified electrocatalysts G/Pani/NiMn1, G/Pani/NiMn2, G/Pani/NiMn3, G/Pani/NiMn4 was investigated using cyclic voltammetry, chronoamperometry, and electrochemical impedance. The kinetic parameters such as diffusion coefficient, Tafel slope, charge transfer coefficient, and surface coverage were calculated to choose the best electrocatalysts toward UEO in alkaline solution. The anodic current of new electrodes achieved about 16 mA.cm−2 at potential of 550 mV (vs. Ag/AgCl). Density functional theory studies (DFT) have been carried out to assess the adsorption energy between polyaniline (Pani) and the metal oxides.