Hierarchically nanostructured materials that combine two or more levels of structuring and that exhibit a combination of useful features have gained considerable interest over recent years. Here, the generation of surface-bound nanofilaments with a high aspect ratio by nanomolding on a nanoporous template surface is described. The filaments, at the same time, carry molecularly imprinted binding sites. The dye fluorescein and the protein myoglobin are used as model templates for imprinting. The surfaces exhibit specific binding as revealed by fluorescence microscopy. The wetting properties of the surfaces depend on the dimensions of the nanofilaments and on the nature of the polymer. it is believed that these materials can potentially be useful for applications in biosensors and biochips.