As part of the Yellowstone River Basin National Water Quality Assessment study, ground-water samples were collected from Quaternary unconsolidated-deposit and lower Tertiary aquifers in the Bighorn Basin of Wyoming and Montana from 1999 to 2001. Samples from 54 wells were analyzed for physical characteristics, major ions, trace elements, nutrients, dissolved organic carbon, radionuclides, pesticide compounds, and volatile organic compounds (VOCs) to evaluate current water-quality conditions in both aquifers. Water-quality samples indicated that waters generally were suitable for most uses, and that natural conditions, rather than the effects of human activities, were more likely to limit uses of the waters. Waters in both types of aquifers generally were highly mineralized, and total dissolved-solids concentrations frequently exceeded the U.S. Environmental Protection Agency (USEPA) Secondary Maximum Contaminant Level (SMCL) of 500 milligrams per liter (mg/L). Because of generally high mineralization, waters from nearly one-half of the samples from Quaternary aquifers and more than one-half of the samples from lower Tertiary aquifers were not classified as fresh (dissolved-solids concentration were not less than 1,000 mg/L). The anions sulfate, fluoride, and chloride were measured in some ground-water samples at concentrations greater than SMCLs. Most waters from the Quaternary aquifers were classified as very hard (hardness greater than 180 mg/L), but hardness varied much more in waters from the lower Tertiary aquifers and ranged from soft (less than 60 mg/L) to very hard (greater than 180 mg/L). Major-ion chemistry varied with dissolved-solids concentrations. In both types of aquifers, the predominant anion changes from bicarbonate to sulfate with increasing dissolved-solids concentrations. Samples from Quaternary aquifers with fresh waters generally were calcium-bicarbonate, calcium-sodium-bicarbonate, and calcium-sodium-sulfate-bicarbonate type waters, whereas samples with larger concentrations generally were calcium-sodium-sulfate, calcium-sulfate, or sodium-sulfate-type waters. In the lower Tertiary aquifers, samples with fresh waters generally were sodium-bicarbonate or sodium-bicarbonate-sulfate type waters, whereas samples with larger concentrations were sodium-sulfate or calcium-sodium-sulfate types. Concentrations of most trace elements in both types of aquifers generally were small and most were less than applicable USEPA standards. The trace elements that most often did not meet USEPA secondary drinking-water standards were iron and manganese. In fact, the SMCL for manganese was the most frequently exceeded standard; 68 percent of the samples from the Quaternary aquifers and 31 percent of the samples from the lower Tertiary aquifers exceeded the manganese standard. Geochemical conditions may control manganese in both aquifers as concentrations in Quaternary aquifers were negatively correlated with dissolved oxygen concentrations and concentrations in lower Tertiary aquifers decreased with increasing pH. Elevated nitrate concentrations, in addition to detection of pesticides and VOCs in both aquifers, indicated some effects of human activities on ground-water quality. Nitrate concentrations in 36 percent of the wells in Quaternary aquifers and 28 percent of the wells in lower Tertiary aquifers were greater than 1 mg/L, which may indicate ground-water contamination from human sources. The USEPA drinking-water Maximum Contaminant Level (MCL) for nitrate, 10 mg/L, was exceeded in 8 percent of samples collected from Quaternary aquifers and 3 percent from lower Tertiary aquifers. Nitrate concentrations in Quaternary aquifers were positively correlated with the percentage of cropland and other agricultural land (non-cropland), and negatively correlated with rangeland and riparian land. In the lower Tertiary aquifers, nitrate concentrations only were correlated with the percentage of cropland. Concentratio