We employed electrospun TiO2 nanofibers (NFs) as a synthetic template to develop three-dimensional (3D) MoS2 nanosheet/TiO2 nanofiber (MoS2/TiO2) heterostructures using a simple hydrothermal method. The prepared 3D MoS2/TiO2 heterostructures exhibited a higher performance in photocatalytic degradation of the dye molecules (rhodamine B and methyl orange) than pure TiO2 NFs under UV light irradiation. The enhanced photocatalytic activity might be attributed to the formation of heterostructures between TiO2 and MoS2, in which MoS2 not only served as electron trapper to improve the separation of photogenerated electron-hole pairs, but also provided a greater number of active adsorption sites for the photodegradation of pollutants. The 3D heterostructure photocatalysts could be easily recycled by sedimentation due to their nanofibrous network structure. The photocatalytic mechanism of 3D MoS2/TiO2 heterostructures was also proposed. (C) 2016 Elsevier B.V. All rights reserved.