A new sorbent for uranium(VI) has been developed by functionalizing ordered mesoporous carbon CMK-5 with 4-acetophenone oxime via thermally initiated diazotization. The sorption of U(VI) ions onto the functionalized CMK-5 (Oxime-CMK-5) was investigated as a function of sorbent dosage, pH value, contact time, ionic strength and temperature using batch sorption techniques. The results showed that U(VI) sorption onto Oxime-CMK-5 was strongly dependent on pH, but to a lesser extent, on ionic strength. Kinetic studies revealed that the sorption process achieved equilibrium within 30 min and followed a pseudo-first-order rate equation. The isothermal data correlated with the Langmuir model better than the Freundlich model. Thermodynamic data indicated the spontaneous and endothermic nature of the process. Under current experimental conditions, a maximum U(VI) sorption capacity was found to be 65.18 mg/g. Quantitative recovery of uranium was achieved by desorbing the U(VI)-loaded Oxime-CMK-5 with 1.0 mol/L HCl and no significant decrease in U(VI) sorption capability of Oxime-CMK-5 was observed after five consecutive sorption-desorption cycles. The sorption study performed in a simulated nuclear industry effluent demonstrated that the new sorbent showed a desirable selectivity for U(VI) ions over a range of competing metal ions.