Effective degradation of organic pollutants in wastewater is of great importance to the environment and human society. TiO2-based electrospun nanofibrous materials combining the properties of the large specific surface area, high aspect ratio, tunable compositions and structures, as well as easy to recycle, show great promise for the efficient removal of organic pollutants. In this Prospective paper, the recent progress in the degradation of organic water contaminants over visible-light-responsive TiO2-based nanofibrous materials is summarized, with emphasis on the strategies for improving the visible-light photocatalytic activity of TiO2-based nanofibrous materials. Finally, the current challenges and future outlook in this field are discussed.