Nanostructured TiO2 thin films were prepared via a low-temperature solution processing. We have previously calculated the degree of supersaturation (s) for TiO2 precursor solution to systematically tailor the development of TiO2 nanostructures in the range of s = 70-200. In this article, we focused more on a lower supersaturation regime (s < 70), from which we were able to obtain various shapes and sizes of nanostructures of TiO2 thin films. A film consisting of rutile phase nanoblades was observed when the degree of supersaturation was s = 15-70. To further lower the supersaturation (s < 15), hydrothermal processing had to be used, for which a film consisting of rutile phase nanorods was obtained. The resulting thin films were evaluated for band gap energies and dielectric properties. The band gap energy for those rutile thin films decreased from 3.22 to 2.99 eV when the supersaturation was lowered from s = 70 to 15. The dielectric constant (k) of the rutile film processed from s = 50 showed the best performance with k similar to 50 at 1 MHz.