A compilation of groundwater-quality data collected as part of two U.S. Geological Survey studies provides a basis for understanding the ambient geochemistry related to geologic setting in the Piedmont and Blue Ridge Physiographic Provinces (hereafter referred to as Piedmont and Mountains Provinces) of North Carolina. Although the geology is complex, a grouping of the sampled wells into assemblages of geologic units described as 'geozones' provides a basis for comparison across the region. Analyses of these two data sets provide a description of water-quality conditions in bedrock aquifers of the Piedmont and Mountains Provinces of North Carolina. Analyzed data were collected between 1997 and 2008 from a network of 79 wells representing 8 regional geozones distributed throughout the Piedmont and Mountains Provinces. This area has experienced high rates of population growth and an increased demand for water resources. Groundwater was used by about 34 percent of the population in the 65 counties of this region in 2005. An improved understanding of the quality and quantity of available groundwater resources is needed to plan effectively for future growth and development. The use of regional geologic setting to characterize groundwater-quality conditions in the Piedmont and Mountains Provinces is the focus of this investigation. Data evaluation included an examination of selected properties and the ionic composition of groundwater in the geozones. No major differences in overall ionic chemistry of groundwater among the geozones were evident with the data examined. Variability in the cationic and anionic composition of groundwater within a particular geozone appeared to reflect local differences in lithologic setting, hydrologic and geochemical conditions, and(or) land-use effects. The most common exceedances of the drinking-water criteria (in accordance with Federal and State water-quality standards) occurred for radon, pH, manganese, iron, and zinc. Radon had the most exceedances, with groundwater from 61 of the 69 sampled wells having activities higher than the U.S. Environmental Protection Agency's proposed maximum contaminant level of 300 picocuries per liter. Overall, the Milton and the Raleigh and Charlotte geozones had the greatest number, eight each, of water-quality properties or constituents that exceeded applicable drinking-water criteria in at least one well. The Eastern Blue Ridge and Felsic intrusive geozones each had seven properties or constituents that exceeded criteria, and the Carolina slate geozone had six. Based on limited data, initial results of statistical comparison tests identified statistically significant differences in concentrations of some groundwater constituents among the geozones. Statistically significant differences in median values of specific conductance and median concentrations of calcium, potassium, sodium, bicarbonate, chloride, silica, ammonia, aluminum, antimony, cadmium, and uranium were identified between one or more geozone pairs. Overall, the groundwater constituents appear to be influenced most significantly by the Inner Piedmont, Carolina slate, and Felsic intrusive geozones. The study data indicate that grouping and evaluating analytical data on the basis of regional geozone setting can be useful for characterizing water-quality conditions in bedrock aquifers of the Piedmont and Blue Ridge Provinces of North Carolina.