Pure siliceous and aluminosilicate mesoporous MCM-41 materials with spherical morphology have been used as supports for Ni deposition accomplished by single-step synthesis and wet impregnation. XRD, TPR and FTIR methods have been used for their characterization and the catalytic performance was evaluated in the reaction of toluene hydrogenation. It was found that the catalytic activity of the Ni modified catalysts depends on the method of their preparation as far as it determines the nature, environment and reducibility of the nickel oxide particles and the metal dispersion after reduction.