Pt catalysts covered with an organosilica layer containing phenyl and/or methyl groups showed higher conversion in the dehydrogenation of cyclohexane, compared with Pt catalysts covered with a silica layer containing no functional groups. Micropores formed in the organosilica layer owing to the decomposition of functional groups by heat treatment resulted in this increase in catalytic activity which is dependent on the functional groups contained in the organosilica layer.