Silica becomes increasingly used in chemical, pharmaceutical, and (nano)technological processes', resulting in an increased demand for well-defined silicas and silica-based materials. The production of highly structured silica from cheap starting materials and under ambient conditions, which is a target for many researchers, is already realized in the formation of diatom biosilica, producing highly hierarchical ordered meso- and macropores silica structures. This notion formed the starting point in our integrative biomolecular and biomimetic study on diatom silicon biomineralization in which we have analyzed silica transformations and structure-direction in polymer-mediated silica syntheses using a combination of (ultra)small-angle X-ray sc...