Microstructured polymer films prepared by photochemical grafting of different polymers were used as restricted reaction areas in silica deposition experiments. Linear and branched poly(alkyleneimines) and poly(allylamine hydrochloride) in pure aqueous or phosphate-containing solutions were used as additives to silica precursor solutions. The silica deposits obtained by spin-coating these solutions onto microstructured polymer films were investigated by scanning electron microscopy and atomic force microscopy. Experiments with poly(alkylene imines) in the silica precursor solution show the deposition of smooth and granular silica structures that closely mimic the natural patterns. The structure formation can be explained by physicochemical processes. Hypotheses that have been made for the natural silification processes can be evaluated on this basis.