Enhanced visible-light-driven photocatalysis of TiO2 nanofibers have been prepared by the electrospinning method combined with a surface nitridation process. The visible-light-driven photocatalytic activity of surface nitrided TiO2 (N-TiO2) nanofibers has been evaluated using rhodamine B indicator, and it was found that the visible-light-driven photocatalytic activity of the electrospun TiO2 nanofibers could be enhanced by nitridation in NH3 atmosphere. The optimal visible-light photocatalytic activity of N-TiO2 nanofibers exceeded that of pure TiO2 nanofibers by a factor of more than 12. The nitridation temperature under NH3 flow was found to play an important part in the performance of N-TiO2 nanofibers, and the optimum temperature is 500 degrees C. Structure, morphology and photoluminescence of these nanofibers were studied by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), scanning electron microscope (SEM) and photoluminescence (PL) spectroscopy. The mechanism of the enhancement of visible-light-driven photocatalytic activity by surface nitridation has been discussed.