In order to further improve the photocatalytic performance of the SiO2/TiO2 composite under visible light irradiation, curcumin-doped SiO2/TiO2 nanocomposites were synthesized via directly incorporating it into the structure of SiO2/TiO2 during the synthesis using an inexpensive and readily available natural pigment (curcumin) as doping agent. The physicochemical properties of SiO2/TiO2 nanocomposites were characterized in detail by X-ray diffraction, transmission electron microscopy, Fourier transform-infrared spectroscopy, N2 adsorption–desorption isotherms, X-ray photoelectron spectroscopy, and UV-vis diffuse reflectance spectroscopy. The results indicate that all SiO2/TiO2 nanocomposites exhibited an anatase phase with a typical mesoporous structure. It was found that the dope of curcumin in the SiO2/TiO2 composite could decrease the crystal size, slightly improve the specific surface areas, significantly enhance the visible light absorption, and effectively narrow the band gap energy from 3.04 to 10(eV). Compared with bare SiO2/TiO2, the curcumin-doped SiO2/TiO2 resulted in enhanced photocatalytic reduction activity for Cr(VI) under visible light irradiation, and the CTS (12) sample with the appropriate content of curcumin of 12 wt % shows the photocatalytic yield reaching 100% within 2.5 hours, which is larger than CT (12) without silica. This could be attributed to the curcumin doping and the synergetic effects of SiO2 and TiO2 in SiO2/TiO2 nanocomposites.