The TiO2/BiOI heterostructured nanofibers were prepared by electrospinning-solvothermal two-step process. The BiOI nanosheets, which owned a thickness of tens of nanometers and an average side length of about 300 nm, were intensive and crossed arranging on the TiO2 nanofibers whose diameter was about 400-550 nm and length was about 15-45 mu m. The absorption edge of TiO2/BiOI heterostructured nanofibers was extended to more than 600 nm in visible-light region and the TiO2/BiOI exhibited enhanced visible-light photocatalytic performance and excellent recyclability compared to the individual TiO2 nanofibers and the BiOI microflowers in the photodecomposition of methylene blue, which was ascribed to nanoscale size heterostructure, narrow energy band, peculiar band gap structures, and porous surface structure.