Hybrid materials based on MCM-41 silica and Y-zeolites with a variable Si/Al ratio and an appropriate countercationic composition were prepared by impregnating inorganic substrates with an organic extract. The organic phase was previously characterized by GC-MS and IRTF, while XRD, SEM, TEM, N2-physisorption, and TPD of NH3 were used to analyze the selected inorganic supports. The effect of size- and shape-selectivity was manifested in MCM-41 and Y-zeolites. Texture results confirm that the extract containing relatively large branched organic molecules is deposited in the internal voids of MCM-41 material and on the outer area of Y-zeolites. In the case of Y-zeolites, the results demonstrate the effect of the SiO2/Al2O3 molar ratio and countercations on the textural properties of the samples.