Nitrogen-doped ZnO nanoparticle-carbon nanofiber composites were prepared using electrospinning. As the relative amounts of N-doped ZnO nanoparticles in the composites were controlled to levels of 3.4, 9.6, and 13.8 wt%, the morphological, structural, and chemical properties of the composites were characterized by means of field-emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). In particular, the carbon nanofiber composites containing 13.8 wt% N-doped ZnO nanoparticles exhibited superior catalytic properties, making them suitable for use as counter electrodes in dye-sensitized solar cells (DSSCs). This result can be attributed to the enhanced surface roughness of the composites, which offers sites for I3- ion reductions and the formation of Zn3N2 phases that facilitate electron transfer. Therefore, DSSCs fabricated with 13.8 wt% N-doped ZnO nanoparticle-carbon nanofiber composites showed high current denisty (16.3 mA/cm2), high fill factor (57.8%), and excellent power-conversion efficiency (6.69%); at the same time, these DSSCs displayed power-conversion efficiency almost identical to that of DSSCs fabricated with a pure Pt counter electrode (6.57%).