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Nitric oxide (NO) pollutant can threaten the regional environment and human health. Solar-powered photocatalytic oxidation method is desirable for NO removal (ppb level) at ambient conditions, but suffers from the unsatisfactory activity and poor selectivity due to the sluggish molecular oxygen activation. Herein, we demonstrate that efficient photocatalytic NO removal can be realized by modulating the defects distribution of amorphous TiO 2 via boron doping. Theoretical calculations and experimental results reveal that H 3 BO 3 modification can refine the structure of surface oxygen vacancies, promoting electron-rich molecular oxygen activation to •OH. Meanwhile, bulk-phase oxygen defects can be filled by free-state B atoms, accelerating the electron transfer via Ti-O-B bonding. Homogeneous boron-doped amorphous TiO 2 achieves about 5 times higher NO removal efficiency (∼50%) than that of amorphous TiO 2 (∼9%) without releasing remarkable NO 2 (selectivity, ∼97%). This study provides a state-of-the-art approach for robust photocatalytic NO removal by engineering the defect distribution. [Display omitted] • The homogeneous boron-doped amorphous TiO 2 was prepared by solvothermal method. • Boron doping can regulate the oxygen defect distribution of amorphous TiO 2. • Boron doping facilitated the molecular oxygen activation to •OH. • Photocatalytic NO removal was enhanced by the cooperation of boron doping and oxygen vacancy. [ABSTRACT FROM AUTHOR]