The present paper describes the catalytic oxidation of urea performed by nickel hydroxide and nickel/cobalt hydroxide modified electrodes by using both electrodeposited films and nanoparticles. The incorporation of Co foreign atoms leads to a slight increase in sensitivity besides the shift in redox process, avoiding the oxygen reaction. Nanostructured Ni80Co20(OH)2 was synthesized by sonochemical route producing 5nm diameter particles characterized by high-resolution transmission electron microscopy (HRTEM) being immobilized onto electrode by using the electrostatic Layer-by-layer technique, yielding attractive modified electrodes for sensor development.