Organosilane-modified mesoporous materials have been prepared under mild and acidic conditions by a solvent evaporation method using C(16)TMABr surfactant as a template. The mesoporous samples synthesized in ethanol solvent by using this evaporation method showed a fully disordered pore system, but those obtained under hydrothermal conditions had highly ordered pores. The chiral salen Mn(Ill) complexes were immobilized on these organosilane-functionalized mesoporous silicas by a grafting method. The catalysts used in the asymmetric epoxidation of styrene and cis-stilbene and the effect of different mesoporous structures on the reactivity was investigated. Similar enantioselectivities were observed by using these heterogenized salen complexes as compared with reaction under homogeneous conditions.