Effective mesoporous nanocrystalline C-doped TiO2 photocatalysts were synthesized through a direct solution-phase carbonization using titanium tetrachloride and diethanolamine as precursors. X-ray photoelectron spectroscopy (XPS) results revealed that oxygen sites in the TiO2 lattice were substituted by carbon atoms and formed a C-Ti-O-C structure. The absorption region of the as-prepared TiO2 was extended to the visible light region in view of the substitution for oxygen sites by carbon atoms. The photocatalytic activities of the as-prepared samples were tested in a flow system on the degradation of NO at typical indoor air levels under simulated solar-light irradiation. The samples showed a more effective removal efficiency than commercial photocatalyst (P25) on the degradation of the common indoor pollutant NO. The parameters significantly affecting the mesoporous structure and removal efficiency on indoor air were also investigated.