Molybdenum diselenide nanosheeticarbon nanofiber (MoSe2/CNF) heterojunctions have been successfully obtained by a facile two-step synthesis route combining an electrospinning technique and solvothermal method. The results show that MoSe2 nanosheets distributed evenly on the carbon nanofibers without aggregation, and the loading amount of MoSe2 could be well controlled by adjusting the reactant concentrations during the solvothermal process for the fabrication of the MoSe2/CNF heterojunctions. The as-prepared MoSe2/CNF heterojunctions exhibited higher photocatalytic activity than pure MoSe2 for the degradation of Rhodamine B (RhB) under visible and infrared light irradiation. The normalized rate constant for the MoSe2/CNF heterojunctions was nearly 3.2 times and 1.6 times higher than that of pure MoSe2 under visible light and infrared light (1.5 W, 980 nm laser) irradiation, respectively. The enhanced photocatalytic activity might be attributed to the formation of heterojunctions, which could improve the separation of photogenerated electrons and holes at the MoSe2/CNF heterojunctions interface. In addition, MoSe2/CNF heterojunctions could be efficiently separated from the solution by sedimentation due to their ultralong one-dimensional and self-supporting structure. Such MoSe2/CNF heterojunctions with a broad-spectrum-response photocatalytic performance might have potential applications in water treatment. (C) 2018 Published by Elsevier Inc.