A permeable reactive barrier (PRB) containing zerovalent iron [Fe(O)] was installed at a former uranium milling site in Monticello, UT. A large-scale column experiment was conducted at the site to test the feasibility of Fe(O) to treat U prior to installing the PRB. Effluents from the field column experiment had pH values near 7.34, moderate decreases in C(IV) and Ca concentrations, and an elevated Fe concentration (27.1 mg/L). In contrast, groundwater exiting the PRB had a pH value of 9.82, decreases in C(IV) and Ca concentrations, and a low concentration of Fe (0.17 mg/L). A geochemical model was used to explain the chemical changes that occurred in both the field column experiment and the PRB. The model simulated the systems by the progressive irreversible dissolution of Fe(O). Modeling results indicated that a longer residence time in the PRB compared with the shorter residence time in the column contributed to the disparate effluent qualities. Prior to modeling, a controlled laboratory column experiment was conducted to help evaluate the dominant chemical mechanisms by which Fe(O) removes U from aqueous solutions. Results of the laboratory column experiment indicated that only a small amount of U could be adsorbed to ferric minerals, and, therefore, this mechanism was not considered in the model.