Two-dimensional (2D) MoS(2)nanosheets vertically supported on TiO2/PVDF flexible fibers have been successfully synthesized by combining electrospinning with a low temperature hydrothermal method without acid. The morphology of the 2D MoS(2)nanosheets could be controlled by adjusting the experimental parameters. The loaded 2D MoS(2)nanosheets can not only broaden the light capture range of TiO2, but also greatly inhibit the recombination rate of photogenerated electron-hole pairs. Due to the synergistic effect between MoS(2)and TiO2, the photocatalytic rate for levofloxacin hydrochloride is about 40 times higher than that for MoS(2)only. Recycle experiments have proved the stability and reusability of TiO2/PVDF@2D MoS(2)nanosheets. The mechanism is investigated by quenching experiments. The results show that the superoxide anion radical (center dot O-2(-)), the hydroxyl radical (center dot OH) and the hole (h(+)) all have contributions to photocatalysis. This work widens the range of materials to synthesize the composites of 2D MoS(2)nanosheets and provides a new and gentle method for preparing flexible large-scale heterostructures for environmental protection.