Silica materials attract an increasing amount of interest in (fundamental) research, and find applications in, for example, sensing, catalysis, and drug delivery.A st he properties of these (nano)materials not only depend on their chemistry but also their size, shape,a nd surface area, the controllable synthesis of silica is essential for tailoringt he materials to specific applications. Advantageously,b ioinspired routes for silica production are environmentally friendly ands traightforward since the formation process is spontaneousa nd proceeds under mild conditions. These strategies mostly employ amine-bearing phosphorylated (bio)polymers. In this work, we expand this principle to supramolecular polymers based on the water-soluble cationic cyanine dye Pinacyanol acetate. Upon assembly in water, these dye molecules form large, polyaminated, supramolecular fibers.T he surfaces of these fibers can be used as ascaffold for the condensation of silicic acid. Controlo ver the ionic strength, dye concentration, and silicic acid saturation yielded silica fibers with ad iameter of 25 nm and as ingle, 4nmp ore. Unexpectedly,o ther unusual superstructures, namely,n ummulites and spherulites, are also observed depending on the ionic strength and dye concentration.T ransmission and scanning electronm icroscopy (TEM and SEM) showedt hat these superstructures are formed by aligned silica fibers. Close examination of the dye scaffold prior silicification using small-angle X-ray scattering (SAXS), and UV/Vis spectroscopy revealed minor influence of the ionic strength and dye concentration on the morphologyo ft he supramolecular scaffold.T otal internal reflection fluorescence (TIRF) during silicification unraveledt hat if the reaction is kept under static conditions, only silica fibers are obtained. Experiments performed on the dye scaffold and silica superstructures evidenced that the marked structurald iversity originates from the arrangemento fs ilica/dye fibers. Under these mild conditions, external force fields can profoundly influence the morphologyo ft he produced silica.