In the present work, iron-functionalized TiO2 nanofibers have been successfully synthesized by an electrospinning system and the resulting nanofibers were characterized using X-ray diffraction, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy and ultra-violet-visible spectroscopy. Microscopic studies revealed that TiO2 nanofibers with average diameters of *60 to 65 nm were formed during the electrospinning process while their diameters increased to *85 to 90 nm by iron functionalization. Moreover, the photocatalytic activities of pristine and iron-functionalized TiO2 nanofibers were measured by photodegradation of methyl orange (MO) as a model dye under visible- light irradiation. It was found that iron-functionalized TiO2 nanofibers extended the light absorption spectrum toward the visible region and noticeably improved the photodegradation of MO under visible-light irradiation. Furthermore, there is an optimum amount of FeCl3 to reach to the highest photocatalytic performance of iron-functionalized TiO2 nanofibers under visible-light.