Arsenic residues in the communities surrounding former smelters remain a public health concern, especially for infants and children. To evaluate environmental exposure among these children, a population-based cross-sectional study was conducted in the vicinity of a former copper smelter in Anaconda, Montana. A total of 414 children less than 72 months old were recruited. First morning voided urine samples and environmental samples were collected for arsenic measurements. The geometric mean of speciated urinary arsenic was 8.6 μg/liter (GSD = 1.7,N= 289). Average arsenic levels of different types of soil ranged from 121 to 236 μg/g, and were significantly related to proximity and wind direction to the smelter site. The same significant relationship was observed for interior dust arsenic. Speciated urinary arsenic was found to be significantly related to soil arsenic in bare areas in residential yards (P < 0.0005). In general, elevated excretion of arsenic was demonstrable and warranted parents' attention to reduce exposure of their children to environmental arsenic.