In this work, zinc oxide/rectorite composites were synthesized by a sol-gel method. The methanol as sacrificial organics could be enhance the adsorption capability and photocatalytic reduction activity of U(VI) onto the zinc oxide/rectorite composites. In addition, the composite still showed the high photoreduction activity after four reaction cycles under visible light irradiation. On the basis of the experimental results and photoluminescence, the enhanced photoreduction activity could be attributed to charge-transfer-complex and the coupling effect of ZnO and rectorite in the composite.