Titanium dioxide nanoparticles have been prepared by solution-phase methods in the three phases that occur naturally, anatase, rutile, and brookite. The amorphous titania starting material was prepared from titanium(IV) iso-propoxide using iso-propanol as solvent and a small quantity of water. The resulting material was treated hydrothermally in an acid digestion vessel at temperatures between 175 °C and 230 °C with different reactants to obtain the three phases or controlled mixtures of two phases. The nanomaterials were characterized by a variety of techniques, including X-ray diffraction, Raman spectroscopy, electron microscopy, dynamic light scattering, and UV-Vis absorbance spectrophotometry. The results illustrate the relation between the properties of the nanoparticles in the colloid, in the powder, and in nanostructured thin films prepared with the materials. A thorough understanding of synthesis methods is essential for the preparation of nanomaterials with tailored structural, morphological, and ultimately, physical properties.