Catalysis, chemical separations, and energy conversion devices often depend on well-defined mesoporous materials as supports or active component elements. Herein, we show that ordered assembled organic surfactant films can directly template porous inorganic solids with surface area exceeding 1000 m(2)/g by infusing the polymers with reactive inorganic vapors, followed by anneal. The specific surface area, pore size, chemical composition, and overall shape of the product material are tuned by choice of the polymer and precursor materials as well as the influsion and postinfusion treatment conditions. X-ray diffraction, infrared spectroscopy, and electron microscopy show that vapor infusion changes both the physical and chemical structure of the starting ordered polymer films, consistent with quantified trends in specific surface area and pore size distribution measured by nitrogen adsorption after film annealing. This method yields porous TiO2 films, for example, that function as an anode layer in a dye-sensitized solar cell.