A study of groundwater chemistry and radionuclide mobility in New Jersey and Maryland was conducted to investigate natural processes that control the mobility of radionuclides in the water-rock system. Groundwater was sampled from two geological units in New Jersey and from six in Maryland. The water sampled was from aquifiers in fractured metamorphic rocks of varying composition and metamorphic grade. In both areas, groundwater chemistry was affected most by aquifier mineralogy and lithology; concentrations of total dissolved U, 226Ra and 222Rn were similarly affected. In evey sample for which measurements were made, dissolved Utotal and 226Ra were present in much lower concentrations than 222Rn when expressed in terms of their radioactivity. On the other hand, the total amount of 222Rn that could be produced in these rocks, given their U contents, is much higher than the concentrations observed in groundwater. Thus, the emanating efficiencies of the aquifer rocks studied must be near 10% or less. Such low emanating efficiencies require that a fraction of the 226Ra in the rock be located close to the water-rock interface so that 222Rn, when produced, can be rapidly and efficiently transferred to the aqueous phase. This condition is established when a similar fraction of the U is in a readily leachable position. No known U or Ra solids were supersaturated in any of the samples. Thus, adsorption processes probably play a role in limiting mobilities of Utotal and 226Ra. Concentrations of Utotal and 226Ra found in the water samples are comparable to those found in experimental studies of adsorption onto mineral surfaces. ?? 1991.