Surface soil and groundwater in Australia have been found to contain high concentrations of arsenic. The relative importance of long-term human exposure to these sources has not been established. Several studies have investigated long-term exposure to environmental arsenic concentrations using hair and toenails as the measure of exposure. Few have compared the difference in these measures of environmental sources of exposure. In this study we aimed to investigate risk factors for elevated hair and toenail arsenic concentrations in populations exposed to a range of environmental arsenic concentrations in both drinking water and soil as well as in a control population with low arsenic concentrations in both drinking water and soil. In this study, we recruited 153 participants from areas with elevated arsenic concentrations in drinking water and residential soil, as well as a control population with no anticipated arsenic exposures. The median drinking water arsenic concentrations in the exposed population were 43.8 mug/L (range, 16.0-73 mug/L) and median soil arsenic concentrations were 92.0 mg/kg (range, 9.1-9,900 mg/kg). In the control group, the median drinking water arsenic concentration was below the limit of detection, and the median soil arsenic concentration was 3.3 mg/kg. Participants were categorized based on household drinking water and residential soil arsenic concentrations. The geometric mean hair arsenic concentrations were 5.52 mg/kg for the drinking water exposure group and 3.31 mg/kg for the soil exposure group. The geometric mean toenail arsenic concentrations were 21.7 mg/kg for the drinking water exposure group and 32.1 mg/kg for the high-soil exposure group. Toenail arsenic concentrations were more strongly correlated with both drinking water and soil arsenic concentrations; however, there is a strong likelihood of significant external contamination. Measures of residential exposure were better predictors of hair and toenail arsenic concentrations than were local environmental concentrations.