We report a facile method for creating nanoscopic oxide structures over large areas that is capable of producing high aspect ratio nanoscale structures with feature sizes below 50 nm. A variety of nanostructured oxides including TiO2, SnO2 and organosilicates are formed using sol-gel and nanoparticle precursors by way of molding with water-soluble polymeric templates generated from silicon masters. Sequential stacking techniques are developed that generate unique 3-dimensional nanostructures with combinatorially mixed geometries, scales, and materials. Applicable to a variety of substrates, this scalable method allows access to a broad range of new thin film morphologies for applications in devices, catalysts, and functional surface coatings. © 2011 American Chemical Society.