NO has caused many serious environmental problems and even seriously threatened human health. The development of a cheap and efficient method to remove NO from the air has become an urgent need. In this paper, a novel nanocomposite metal-semiconductor photocatalyst Bi-Bi2Ti2O7/CaTiO3 was prepared. Compared to the original Bi2Ti2O7/CaTiO3, the modification by the metal Bi increased its photocatalytic activity from 25% to 64% under visible light irradiation. The improved photoactivity owns to the SPR effect and the electron capture effect of Bi metals in metal-semiconductor loaded systems improving the separation efficiency of electron-hole pairs and significantly improving the light absorption capacity of the composite photocatalyst. The capture experiment of active species showed that •OH, •O2−, h+ and e− are the main active species in the photocatalytic conversion of NO. This work provides new insights into the conformational relationships of Ti-based photocatalysts for NO removal.