Carbon nanofiber (CNF) composites coated with spindle-shaped Fe2O3 nanoparticles (NPs) are fabricated by a combination of an electrospinning method and a hydrothermal method, and their morphological, structural, and chemical properties are measured by field-emission scanning electron microscopy, transmission electron microscopy, Xray diffraction, and X-ray photoelectron spectroscopy. For comparison, CNFs and spindle-shaped Fe2O3 NPs are prepared by either an electrospinning method or a hydrothermal method, respectively. Dye-sensitized solar cells (DSSCs) fabricated with the composites exhibit enhanced open circuit voltage (0.70 V), short-circuit current density (12.82 mA/cm2), fill factor (61.30%), and power conversion efficiency (5.52%) compared to those of the CNFs (0.66 V, 11.61 mA/cm2, 51.96%, and 3.97%) and spindle-shaped Fe2O3 NPs (0.67 V, 11.45 mA/cm2, 50.17%, and 3.86%). This performance improvement can be attributed to a synergistic effect of a superb catalytic reaction of spindle-shaped Fe2O3 NPs and efficient charge transfer relative to the one-dimensional nanostructure of the CNFs. Therefore, spindle-shaped Fe2O3-NPcoated CNF composites may be proposed as a potential alternative material for low-cost counter electrodes in DSSCs.