In nature, mineralization of hard tissues occurs due to the synergistic effect of components present in the organic matrix of these tissues, with templating and catalytic effects. In Suberites domuncula, a well-studied example of the class of demosponges, silica formation is mediated and templated by an axial proteinaceous filament with silicatein-alpha, one of the main components. But so far, the effect of other organic constituents from the proteinaceous filament on the catalytic effect of silicatein-alpha has not been studied in detail. Here we describe the synthesis of core-shell TiO2@SiO2 and TiO2@ZrO2 nanofibers via grafting of silicatein-alpha onto a TiO2 nanowire backbone followed by a coassembly of silintaphin-1 through its specifically interacting domains. We show for the first time a linker free, one-step funtionalization of metal oxides with silicatein-alpha using glutamate tag. In the presence of silintaphin-1 silicatein-alpha facilitates the formation of a dense layer of SiO2 or ZrO2 on the TiO2@protein backbone template. The immobilization of silicatein-alpha onto TiO2 probes was characterized by atomic force microscopy (AFM), optical light microscopy, and high-resolution transmission electron microscopy (HRTEM). The coassembly of silicatein-alpha and silintaphin-1 may contribute to biomimetic approaches that pursue a controlled formation of patterned biosilica-based biomaterials.