Highly ordered mesoporous organic-inorganic hybrid silica thin films with covalently bonded, positively chargeable -NH2 terminal groups were synthesized by evaporation induced self-assembly of tetraethoxysilane, 3-aminopropyl-triethoxysilane, and a nonionic surfactant under acid conditions and characterized using TEM, GISAXS, FTIR, SAW-based N2 sorption, and TGA.