A BaSnO3 sample loaded with CdS quantum dots (CdS QDs/BaSnO3) was prepared by an electrostatic self-assembly method. The obtained CdS QDs/BaSnO3 nanocomposites exhibited an efficient visible light utilization and photocatalytic NO oxidation activity. The experimental results revealed that the loading of CdS QDs tremendously improved the light absorption range and the separation efficiency of photogenerated electron-hole pairs. In-situ DRIFTS tests demonstrated that the introduced Cd2+ could provide new active sites for NO adsorption and activation. Simultaneously, the EPR test showed that the introduction of CdS QDs induced the generation of ·O2–, which was conducive to promoting the deep oxidation of NO. This study provides a facile and effective synthesis method and strategy for improving the photocatalytic NO removal efficiency while significantly suppressing the NO2 concentration.