MCM-41 materials modified by Al, Zr and Ti were used as supports for the preparation of the NiW hydrodenitrogenation (HDN) catalysts. The modified supports, with highly dispersed Al, Zr and Ti species and without loss of the MCM-41 characteristics, can be prepared by a postsynthetic method. The incorporation of Al, Zr and Ti can enhance the density of acid sites on the modified MCM-41, so as to increase the density of acid sites and even enhance the dispersion of Ni, W species on the corresponding catalysts. The HDN results showed that the incorporation of Al, Zr and Ti can increase the HDN activity of the catalysts and the activity followed the order of Ni/W/Al > Ni/W/Zr > Ni/W/Ti > Ni/W. The high HDN activity of Ni/W/Al ascribed to the high density of acid sites and the well dispersion of the Ni and W species on the catalyst.