Graphene/carbon composite nanofibers (CCNFs) with attached TiO2 nanoparticles (TiO2-CCNF) were prepared, and their photocatalytic degradation ability under visible light irradiation was assessed. They were characterized using scanning and transmission electron microscopy, X-ray diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy, and ultraviolet-visible diffuse spectroscopy. The results suggest that the presence of graphene embedded in the composite fibers prevents TiO2 particle agglomeration and aids the uniform dispersion of TiO2 on the fibers. In the photodegradation of methylene blue, a significant increase in the reaction rate was observed with TiO2-CCNF materials under visible light. This increase is due to the high migration efficiency of photoinduced electrons and the inhibition of charge-carrier recombination due to the electronic interaction between TiO2 and graphene. The TiO2-CCNF materials could be used for multiple degradation cycles without a decrease in photocatalytic activity. (C) 2012 Elsevier Ltd. All rights reserved.