Coconut husk activated carbon (CHAC) was used as an adsorbent to remove hexavalent uranium (U(VI)) from aqueous solutions by adsorption. Batch experiments were conducted to investigate the effects of contact time, pH, initial U(VI) concentration, and adsorbent dosage on U(VI) adsorption. The adsorption process reached an equilibrium state after 150 min. The uptake of U(VI) was highly pH dependent, and the optimum adsorption was at near-neutral pH. High U(VI) removal efficiencies could be achieved by increasing CHAC dosages. The uranium adsorption capacity increased with increasing initial U(VI) concentrations. Above a certain point, any further increase in initial U(VI) concentration produced no significant change in uranium adsorption capacity. Langmuir and Freundlich models were employed to describe the adsorption isotherm of U(VI) by CHAC. The Langmuir model fitted the equilibrium data better than the Freundlich isotherm. The maximum U(VI) adsorption capacity of CHAC was 6.67 mg/g. Kinetics data were also examined in terms of adsorption kinetics using pseudo-first-order and pseudo-second-order kinetic models. The results suggested that the adsorption process followed the pseudo-second-order kinetics well. In summary, CHAC had significant potential for the removal of U(VI) from aqueous solutions.