A novel molecularly hybridized polyethylene/silica composite thin film was obtained by the gas-phase polymerization of ethylene with a titanocene-mounted mesoporous silica layer on a mica plate with mesoscopic pores arranged on the film surface. However, the use of titanocene-mounted hexagonal domains of mesoporous silica on a glass plate for the gas-phase polymerization of ethylene resulted in the formation of an islanded polyethylene/silica hybridized material.