A layered crystalline titanate (T2CT) [Anthony and Dosch, US Patent 5 177 045 (1993)] is intercalated with silicon-amine compounds, such as 3-aminopropyltrimethoxysilane and n-[3-(trimethoxysilyl)propyl] ethylenediamine. N-alkylamine is used as a secondary swelling agent to adjust the amount of silicon-amine intercalating into T2CT. Molybdenum and nickel are loaded into siliconamine intercalated T2CT by impregnation. Hydrogenation of pyrene, hydrodesulfurization of dibenzothiophene, and hydrodenitrogenation of quinoline are used to study the catalytic activity of the NiMo catalysts. The most active NiMo catalysts was activated by calcination and then sulfiding. The NiMo/pillared T2CT catalysts are more active than a commercial catalyst (Shell 324M) for hydrogenation of pyrene, while the activities of the NiMo/pillared T2CT catalysts for hydrodesulfurization and hydrodenitrogenation are similar to those of Shell 324M. The amount of silicon relative to titanium of the pillared T2CT, used as supports, has a significant effect on the catalytic activities and physical properties of the supports.