Carbon-modified titanium dioxide nanoparticles (C:TiO 2 NPs) have been synthesized by ultrasonic nebulizer spray pyrolysis (USP) and pneumatic spray pyrolysis (PSP) techniques. HRTEM on the NPs shows difference in lattice spacing in the NP structures prepared by the two methods-2.02Å for the USP NPs and an average of 3.74Å for the PSP NPs. The most probable particle sizes are 3.11 nm and 5.5 nm, respectively. Raman spectroscopy supported by FTIR confirms the TiO 2 polymorph to be anatase with the intense phonon frequency at 153 cm −1 blue-shifted from 141 cm −1 ascribed to both carbon doping and particle size. A modified phonon confinement model for nanoparticles has been used to extract phonon dispersion and other parameters for anatase for the first time. Electronic measurements show "negative conductance" at some critical bias voltage, which is characteristic of n-type conductivity in the carbon-doped TiO 2 NPs as confirmed by the calculated areas under the I-V curves, a property suited for solar cell applications. Practical solar cells built from carbon-doped TiO 2 electrodes show up to 1.5 times improvement in efficiency compared to pure TiO 2 electrodes of similar construction.