Long titanate nanofibers (typically 10–500 μm in length and 20–50 nm in diameter) were successfully prepared in high yield by the direct hydrothermal processing using natural rutile as a starting material. Fourier transform infrared spectroscopy, transmission electron microscopy, energy dispersive x-ray spectroscopy, electron diffraction, and x-ray diffraction demonstrated that the as-synthesized nanofibers presumably consisted of sodium hydrogen trititanate [(Na,H)2Ti3O7, e.g., Na0.4H1.6Ti3O7] including some hexatitanate-type defects [(Na,H)2Ti6O13]. A partial topotactic condensation model explained their nanostructure well. Although the as-synthesized fibers are defective, they can be cured by a post-heat-treatment in air. The direct hydrothermal treatment for natural rutile will be a promising low-cost process for one-dimensional nanomaterials, which can act not only as a reaction step but also as a purification step.