Coral-like TiO 2−δ microstructures with high surface area were synthesized by a simple hydrothermal method, followed by thermal treatment in a N 2 atmosphere. The introduction of oxygen vacancies (OVs) to TiO 2 significantly improved light absorption and inhibited the recombination of photogenerated charge carriers. Then, multiwalled carbon nanotubes (CNTs) and N-doped carbon quantum dots (N-CQDs) were decorated on the surface of coral-like TiO 2−δ microstructures. The CNTs could greatly improve the separation and transfer efficiency of photogenerated charge carriers, while the N-CQDs could further extend light absorption to longer wavelengths, including the IR region. According to the results of electron spin resonance (ESR) spectroscopy, the introduction of OVs to TiO 2−δ and surface modification with CNTs and N-CQDs promoted the generation of • O 2 − and • OH active species. The formation of • O 2 − and • OH active species on the surface of TiO 2−δ /CNTs/N-CQDs played an important role in the deep oxidation and selective conversion of NO into nitrate. Density functional theory calculations revealed the adsorption and reaction sites for H 2 O and O 2 separately in space over the surface of TiO 2−δ /CNTs/N-CQDs. Namely, the reaction sites of H 2 O and O 2 are on the surface of TiO 2−δ and CNTs, respectively. The electron transfer from TiO 2−δ to CNTs was further verified through the differential charge density. This study demonstrates a straightforward approach for designing full-spectrum-responsive photocatalysts with high efficiency, stability, and selectivity for NO removal.