The distribution and movement of arsenic was investigated on the Aberjona watershed in eastern Massachusetts for the purpose of identifying where and by what processes present and past human exposures to this element could have occurred. It was found that although most of the arsenic was originally released in the headwaters of the watershed, extensive migration had occurred, and the potential for human exposure existed far from designated hazardous waste sites. Both surface water and groundwater were found to be important transport pathways; arsenic moved between these two media at several locations in the watershed, with hydrology and concomitant redox, sorption, and alkylation processes determining the observed patterns of arsenic movement. These findings demonstrate that risk assessments or remedial investigations restricted to designated sites or properties in a watershed may yield both an inaccurate picture of the overall risks presented by a chemical and a less-than-optimum focus for remedial efforts. Since total recovery of the arsenic on this watershed is probably not feasible, cost-effective management will also depend on an adequate understanding of arsenic biogeochemistry and hydrologic transport processes at the watershed scale. Because the Aberjona Watershed is typical of many urban, industrialized areas, these results suggest that the whole watershed often defines the appropriate unit for investigation of chemical contamination in the environment.