Nanofabrication based on biological templates has attracted considerable interest because of its applicationsi n materials science and biomedicine. Herein, af acile method is reported for the synthesis of well-definedT iO 2 nanofibers by using as imple N-(9-fluorenylmethoxycarbonyl)-protected phenylalanine-phenylalanine-aspartic acid tripeptide (Fmoc-Phe-Phe-Asp-OH, Fmoc-FFD) as the template. Compared with other synthetic methods of inorganicn anomaterials, these self-assembling peptides could control the structure and the catalytic activityo ft he synthesized nanomaterials produced under mild synthetic conditions. The as-synthesized peptide-TiO 2 hybrid nanofibers and the calcined TiO 2 nanofibersw ere characterizedb yu sing transmission electron microscopy (TEM), scanning electron microscopy (SEM), circular dichroism (CD) spectroscopy,a nd X-ray diffraction (XRD).T he resultss how that well-defined TiO 2 nanofibers could form when the pH of the peptide solution was 5-7, whereas nanoparticles formed when the pH was 8. Moreover,t he peptide-templated TiO 2 nanofibers showedi mprovedp hotocatalytic activity for the degradation of methyl orange (MO). Finally,t he photocatalytic activity of the TiO 2 could be controlled by adjusting the pH of the peptides olution during the syntheticp rocess.