A series of carbon fiber based ZrO2–TiO2 (Zr/Ti/CF) nanocomposites were synthesized with carbon fiber loadings from 3 to 10 wt% by the solvothermal method. For comparison, Zr/Ti, Ti/CF and Zr/CF catalysts were also synthesized. The resultant samples were characterized by SEM, XPS, XRD, FT-IR, and UV–Vis spectroscopy. XRD results revealed that the catalysts were having anatase TiO2 with excellent crystallinity. SEM studies show that the surface of Zr/Ti/CF/10 catalyst has round-shaped grains with dimensions in the range of 16–20 nm. Under UV-A and visible light irradiation, Zr/Ti/CF catalyst exhibited excellent photocatalytic performance for Orange II degradation when compared with Zr/Ti, Zr/CF and Ti/CF. The enhancing efficiency was attributed to the synergetic effect of adsorption–photocatalysis and to the reduction of the band gap energy.