Ti-Containing MCM-41 materials were organically modified by employing an organosilane with a bridging organic group between two Si, and employed as catalysts for olefin oxidation using H2O2 as oxidant. The incorporation of a bridging organic group resulted in an increase in d spacing, in contrast to the modification with organosilane having terminal alkyl group, which provides decreased d spacing. High hydrophobicity of organically bridged Ti-MCM-41 materials led to high selectivity to epoxide by depressing allylic oxidation.