Aluminated mesoporous silica was prepared by multiple post-grafting of alumina onto uniform mesoporous SiO 2 , which was assembled from monodisperse SiO 2 microspheres. Hydrodesulfurization (HDS) catalyst was prepared by loading Ni and Mo active components onto the aluminated uniform mesoporous SiO 2 , and its HDS catalytic performance was evaluated using hydrodesulfurization of dibenzothiophene as the probe reaction at 300°C and 6.0 MPa in a tubular reactor. The samples were characterized by N 2 physisorption, scanning electronic microscopy, Fourier transform infrared spectrum, X-ray diffraction (XRD), temperature-programmed desorption of ammonia (NH 3 -TPD), 27 Al nuclear magnetic resonance ( 27 Al-NMR) and high-resolution transmission electron microscopy (HRTEM). The results showed that the Si-OH group content of SiO 2 was mainly dependent on the pretreatment conditions and had significant influence on the activity of the NiMo catalyst. The surface properties of the aluminated SiO 2 varied with the Al 2 O 3 -grafting cycles. Generally after four cycles of grafting, the aluminated SiO 2 behaved like amorphous alumina. In addition, plotting of activity of NiMo catalysts supported on aluminated mesomacroporous silica materials against the Al 2 O 3 -grafting cycle yields a volcano curve.