The present work aims at obtaining a suitable and selective catalyst for catalytic dehydrogenation reactions through designing pore structures of silica-containing alumina nanocomposites by optimizing silica content in the structure. In this trend, series of silica-containing alumina nanocomposites with different molar ratios Al 2 O 3 /SiO 2 were prepared by the solvothermal method. According to surface characterization of silica-containing alumina nanocomposites, the sample with the highest molar ratio of Al 2 O 3 /SiO 2 (2.06) showed mesoporous structure with selective pore sizes of 3.7 and 4.6 nm. In addition, it had a high surface area value of 308 m 2 /g. Furthermore, SEM and TEM images of the same sample showed ultra fine sized particles in the nano size (7-17 nm). Dehydrogenation catalysts, as developed structures, were then achieved by loading 0.6 wt.% platinum metal over the prepared nanocomposites. Performances of the prepared nanocatalysts were investigated via the dehydrogenation of a model compound namely; cyclohexane. Experimental results showed that the Pt catalyst supported on the silica-containing alumina nanocomposites with the highest molar ratio of Al 2 O 3 /SiO 2 , is an efficient and selective catalyst toward the dehydrogenation reaction. This was revealed in terms of 100% selectivity of this catalyst toward the conversion of cyclohexane at all ranges of temperatures with the conversion reaction being temperature dependent. Practically, the total conversion of cyclohexane increased with increasing reaction temperature and reached 100% at 450°C while the prepared catalyst demonstrated absolute selectivity. ª 2014 Production and hosting by Elsevier B.V. on behalf of Egyptian Petroleum Research Institute.