A study on the electrosorption of uranium ions onto a porous activated carbon fiber (ACF) was performed to treat uraniumcontaining lagoon sludge. The result of the continuous flow-through cell electrosorption experiments showed that the applied negative potential increased the adsorption kinetics and capacity in comparison to the open-circuit potential (OCP) adsorption for uranium ions. Effective U(VI) removal is accomplished when a negative potential is applied to the activated carbon fiber (ACF) electrode. For a feed concentration of 100 mg/L, the concentration of U(VI) in the cell effluent is reduced to less than 1 mg/L. The selective removal of uranium ions from electrolyte was possible by the electrosorption process.