In this article, novel types of Bi2S3-Au heterostructures are fabricated through rationally controlling the growth atmosphere. Under argon, Au nanoparticles are preferentially deposited onto the tips of Bi2S3 nanorods to form Bi2S3-Au dumbbell heterostructures. In contrast, because of the etching effect by amine, Au nanoparticles are randomly anchored onto the surface of nanorods to form Bi2S3-Au nanocorns in the presence of oxygen. Furthermore, the size of gold nanoparticles can be controlled through adjusting the concentration of reaction precursors. Bi2S3-Au dumbbells show superior activity for the photodegradation of organic pollutants and an enhanced photoresponse compared to the Bi2S3-Au nanocorns. The significantly improved photocatalytic performance of Bi2S3-Au dumbbells is ascribed to the more efficient charge separation compared to that of Bi2S3-Au nanocorns. These heterostructures composed of environmentally friendly elements are expected to be promising for applications in the field of clean energy.