Metal sulfide semiconductors, such as molybdenum disulfide (MoS 2 ) and bismuth trisulphide (Bi 2 S 3 ), are of considerable interest for their excellent applications in photocatalysis and in many other fields. However, the controllable synthesis of MoS 2 /Bi 2 S 3 hybrid nanostructures remains a challenge. In this study, we report a unique sacrificial templating strategy for preparing layer-controlled MoS 2 on three-dimensional (3D) Bi 2 S 3 micro-flowers. For this approach, Bi 2 S 3 was utilized as a sacrificial template to regulate the ion exchange, and the dosage of molybdenum was adjusted to tune the dynamic formation, thus converting the MoS 2 nanosheets on the Bi 2 S 3 micro-flowers from monolayer to multilayer. Such a 3D flower-like hybrid nanostructure enables MoS 2 /Bi 2 S 3 to exhibit adsorption-promoted photocatalysis under visible light irradiation, especially for the excellent photodegradation of low-concentration organic pollutants, for example, azo dye and atrazine. The observed superiority of the 3D MoS 2 /Bi 2 S 3 was mainly attributed to the increased mass transfer, robust light-harvesting capacity, improved charge separation, lower oxygen-activation barrier and enhanced active oxygen yield. Our findings are of interest for the development of novel S-based photocatalysts and provide a new opportunity to efficiently remove low-concentration refractory pollutants.