Arsenic concentrations from 20,450 domestic wells in the U.S. were used to develop a logistic regression model of the probability of having arsenic > 10 µg/L (“high arsenic”), which is presented at the county, state, and national scales. Variables representing geologic sources, geochemical, hydrologic, and physical features were among the significant predictors of high arsenic. For U.S. Census blocks, the mean probability of arsenic > 10 µg/L was multiplied by the population using domestic wells to estimate the potential high-arsenic domestic-well population. Approximately 44.1 M people in the U.S. use water from domestic wells. The population in the conterminous U.S. using water from domestic wells with predicted arsenic concentration > 10 µg/L is 2.1 M people (95% CI is 1.5 to 2.9 M). Although areas of the U.S. were underrepresented with arsenic data, predictive variables available in national datasets were used to estimate high arsenic in unsampled areas. Linking predictive modeling to private well use information nationally, despite the uncertainty, is beneficial for broad screening of the population at risk from elevated arsenic in drinking water from private wells. This dataset represents modeled probabilities of arsenic > 10 micrograms per liter in domestic wells in the U.S.