The reactive transport of U(VI) in a shallow alluvial aquifer beneath a former U(VI) mill located near Naturita, CO, was simulated using a surface complexation model (SCM) to describe U(VI) adsorption. The groundwater had variable U(VI) concentrations (0.01–20 μM), variable alkalinity (2.5–18 meq/L), and a nearly constant pH equal to 7.1. U(VI) K_D values decreased with increasing U(VI) and alkalinity, and these parameters were more important than sediment variability in controlling K_D values. Reactive transport simulations were fit to the observed U(VI) and alkalinity by varying the concentration of U(VI) and alkalinity in recharge at the source area. Simulated K_D values varied temporally and spatially because of the differential transport of U(VI) and alkalinity and the nonlinearity of U(VI) adsorption. The model also simulated the observed U(VI) tailing, which would not be expected from a constant K_D model. The simulated U(VI) concentrations were sensitive to the recharge flux because of the increased flux of U(VI) to the aquifer. The geochemical behavior of U(VI) was most sensitive to the alkalinity and was relatively insensitive to pH.