Photosensitization is a promising way to make UiO-66 visible light responsive. In this work, zirconium (Zr) precursors and synthetic methods (solvent-assisted or nonsolvent-assisted) were found to significantly affect the electric charge and the defect sites of UiO-66. UiO-66 with enhanced adsorption and photosensitized photocatalytic ability was then obtained. When ZrOCl2 center dot 8H(2)O was applied as Zr-precursor in a nonsolvent method, defect rich UiO-66 (UiO-OCl-N) was achieved with higher Cr(VI) adsorbing ability and improved photosensitized photocatalytic ability. Moreover, with the coexistence of Rhodamine B in Cr(VI) solution, photocatalytic performance of UiO-66 can be further enhanced.