The unmined Coles Hill U deposit in the Virginia Piedmont represents a unique natural laboratory for studying the long-term containment of U by phosphate minerals. The primary ore assemblage consists of coffinite and apatite and is hosted in foliated granite. Geochemical and mineralogical studies of the weathered bedrock and soils developed over the primary ore body indicate that U transport is inhibited by the precipitation of meta-autunite group minerals. The lower part of the profile, which consists of ground water saturated saprolite, contains 1400 mg/kg U (in the solid). This concentration is 1.5 times greater than the mean ore grade of the deposit, indicating that the saprolites are enriched in U relative to the underlying primary ore. Uranium within the saprolite is dominantly associated with 10 to 500 μm long, tabular crystals of (Ba, Ca, Sr) meta-autunite. Ground waters from this zone contain less than 14 μg/L dissolved U suggesting that the U(VI) phosphate minerals present are capable of controlling dissolved U concentrations at values lower than the US-EPA maximum contaminant level (30 μg/L). Mineralogical characterization of the unsaturated soil horizons indicate that geochemical conditions in these zones are not conducive to U stabilization by meta-autunite mineralization. In the vadose zone U is primarily associated with Al phosphate (crandallite) and with P adsorbed or coprecipitated with iron oxide mineral coatings. Geochemical gradients suggest that significant amounts of U have been leached from the vadose zone by infiltrating fluids and reprecipitated below the water table, where the activity ratio of dissolved phosphate to carbonate increases. Based on regional weathering rates, the processes responsible for stabilization of U within the Coles Hill system are estimated to have been active for hundreds of thousands of years.