[en] Highlights: • A novel surface regulation strategy is developed to modify BiOBr flowers. • More active imprinting sites are constructed on the surface of BiOBr. • The sugar molecule-regulated BiOBr exhibits an enhanced photocatalytic ability. -- Abstract: Bismuth oxybromide (BiOBr) is a representative bismuth photocatalytic material that has been extensively investigated and applied in photodegradation and photoelectrochemistry due to its unique layered structure. However, poor oxidative ability of photoexcited holes from BiOBr causes low degradation rate of refractory pollutants, such as phenol. Thus, developing a general strategy for regulating surface band structure and obtaining photoexcited holes with strong oxidative ability is necessary in BiOBr. We developed a novel surface regulation strategy of BiOBr in this study to obtain active imprinting sites for improving its photocatalytic activity. Various kinds of sugars are selected to regulate surface structures for obtaining the positive-surface valence band maximum of BiOBr and active hydroxyl imprinting sites and then improving photooxidative activities toward organic pollutants and strong photoelectric responses. Among them, maltose-regulated BiOBr with additional hydroxyl active sites exhibits the maximum photodegradation rate of phenol and methylene blue. The valence band of BiOBr was maximally increased after the surface recombination of sugar. This novel surface regulation strategy is a facile, general, and effective approach for improving the photocatalytic activity of BiOBr flowers to provide a new route for modifying surface structure of other photocatalysts and improving their activity.