Mo and NiMo oxides supported on gamma-Al203-Zr02 were successful one-pot synthesized and characterized by XRF, XRD, N2 sorption, UVVISDRS and Zeta Potential. The sulfide catalysts were evaluated between 240 and 300 degrees C in the thiophene HDS, used as a model reaction. XRD data evidenced the presence of gamma-Al2O3 in the obtained solids, with its crystallinity being reduced with the incorporation of Zr and metallic species. XRD data also indicated that Zr, Ni and Mo were highly dispersed on the support. N-2 sorption and UVVISDRS analyses showed that the one-pot synthesis procedure led to Mo and NiMo supported solids with high SBET areas and to Mo species with a low polymerization degree. Zeta Potential and H-2-TPR analyses showed the influence of Ni and Zr in the Mo redox properties that contributed to the well HDS performance of the studied catalysts. The NiMo-gamma-Al2O3-ZrO2 catalysts prepared in this work by a onepot synthesis procedure, especially the NiM0/80A20Z, presented specific activities (QTOF) in the same order that those obtained for a commercial and for a traditional catalyst prepared by wet impregnation. The used one-pot method reduced the synthesis steps, minimizing the preparation time and the energy consumption. (C) 2014 Elsevier B.V. All rights reserved.