In this work, the Bi1-xNdxFeO3 (x = 0, 0.05, 0.10, and 0.15) nanofibers have been successfully synthesized by electrospinning. These nanofibers were about 200–300 nm in diameter and up to several hundred microns in length. The X-ray diffraction data showed that the structure of the Bi1-xNdxFeO3 nanofibers was transformed from the rhombohedral to pseudotetragonal phase by the increasing Nd doping content. Optical absorption study showed that the Nd-doping resulted in a significant red shift, and the bandgap energy of the Bi1-xNdxFeO3 nanofibers was 2.25, 2.15, 2.07, and 2.03eV, respectively. The magnetic hysteresis loops of the nanofibers possessed wasp-waisted shape, and the saturation magnetization was enhanced significantly with the increasing Nd content, which may be a potential candidate for nanoscale components in transformers and inductors.