The role of 3D alumina foam support (Al-F) and titania-modified alumina foam support (Al-F-Ti-X, where X represents the weight ratio of Al-F/TiO2) on the dispersion and catalytic activity of NiMo metals in the hydrodesulfurization (HDS) reaction of dibenzothiophene was studied in a batch reactor. The catalysts were characterized by X-ray diffraction (XRD), N-2 adsorption desorption isotherm, field emission scanning electron microscopy (FESEM), Fourier-transform infrared (FTIR) spectroscopy, temperature-programmed desorption (TPD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The Al-F and Al-F-Ti-10 dispersed the active metals better than the other supports, and more MoS2 was formed on the Al-F-Ti-10 support. TiO2 incorporation into Al-F decreased its surface area but also increased its surface acidity. The Al-F catalyst exhibited a relatively higher HDS activity (81% DBT conversion) over the conventional gamma-Al2O3 -supported NiMo catalyst (72% conversion). The modified Al-F-Ti-10 catalyst demonstrated the highest HDS activity of 97% DBT conversion after 4 h of reaction.