Our previous work demonstrated the fabrication of the NiO nanoparticle-nanographitic flake composite through a direct current (DC) electrophoretic deposition (EPD) process. The composite was used as a catalyst layer having a low onset voltage in ethanol electro-oxidation. This paper presents a new catalyst material fabricated through pulsed EPD, which permitted to acquire a higher efficiency of ethanol electro-oxidation when compared to the catalyst layer fabricated by the DC EPD. The reason behind the enhancement of the performances of the catalyst layers fabricated using the pulsed EPD is the selective deposition of low-weight NiO nanoparticles on nanographitic flakes causing a reduction in the deposition of agglomerated NiO nanoparticles and therefore an enhancement in the efficiency of the ethanol electro-oxidation.