As part of the National Water-Quality Assessment Program of the U.S. Geological Survey, an assessment of 60 volatile organic compounds (VOCs) in untreated, ambient groundwater of the conterminous United States was conducted based on samples collected from 2948 wells between 1985 and 1995. The samples represent urban and rural areas and drinking-water and nondrinking-water wells. A reporting level of 0.2 μg/L was used with the exception of 1,2-dibromo-3-chloropropane, which had a reporting level of 1.0 μg/L. Because ambient groundwater was targeted, areas of known point-source contamination were excluded from this assessment. VOC concentrations generally were low; 56% of the concentrations were less than 1 μg/L. In urban areas, 47% of the sampled wells had at least one VOC, and 29% had two or more VOCs; furthermore, U.S. Environmental Protection Agency drinking-water criteria were exceeded in 6.4% of all sampled wells and in 2.5% of the sampled drinking-water wells. In rural areas, 14% of the sampled wells had at least one VOC; furthermore, drinking-water criteria were exceeded in 1.5% of all sampled wells and in 1.3% of the sampled drinking-water wells. Solvent compounds and the fuel oxygenate methyl tert-butyl ether were among the most frequently detected VOCs in urban and rural areas. It was determined that the probability of finding VOCs in untreated groundwater can be estimated on the basis of a logistic regression model by using population density as an explanatory variable. Although there are limitations to this national scale model, it fit the data from 2354 wells used for model development and adequately estimated the VOC presence in samples from 589 wells used for model validation. Model estimates indicate that 7% (6−9% on the basis of one standard error) of the ambient groundwater resources of the United States probably contain at least one VOC at a reporting level of 0.2 μg/L. Groundwater is used in these areas by 42 million people (35−50 million based on one standard error); however, human exposure to VOCs from this ambient groundwater is uncertain because the quality of the finished drinking water is generally unknown.