Highly effective utilization of solar light is very important for water treatment via photocatalysis. To achieve this goal, we designed and synthesized an efficient full-spectrumresponse photocatalyst based on MoSe 2 /TiO 2 nanofibers. Ultrathin MoSe 2 nanosheets with controllable size and density were evenly grown on electrospun TiO 2 nanofibers by a simple solvothermal method. Under full spectrum irradiation, the photocatalytic reaction rates of MoSe 2 /TiO 2 nanofibers for the removal of rhodamine B, tetracycline hydrochloride and K 2 Cr 2 O 7 aqueous solutions were 7.7, 9.0, and 7.6 times higher than pure MoSe 2 , and were 2.4, 1.4, and 38 times higher than pure TiO 2 , respectively. The loading amounts of MoSe 2 nanosheets have strong effects on their performance. All ultraviolet, visible, and near-infrared light collected by the heterostructures can be well converted to strong oxidizing •O 2 − and •OH and reducing electrons, which are useful active species for removing water pollutants of organics or reducible metal ions. The uniform interface contact and hierarchical heterostructure improved their charge separation and transfer properties, whereas their ultralong one-dimensional and nanofibrous network structure ensured their excellent reusable property. This work presents a new vision in designing full-spectrum-response photocatalysts with efficient and reusable properties.