Natural occurrences of ground water with moderate (10 to 50 micrograms per liter) to high (greater than 50 micrograms per liter) concentrations of arsenic are common throughout much of the Western United States. High concentrations of arsenic are generally associated with one of four geochemical environments: (1) basin-fill deposits of alluvial-lacustrine origin, particularly in semiarid areas, (2) volcanic deposits, (3) geothermal systems, and (4) uranium and gold-mining areas. These findings are based on an extensive literature review, compilation of unpublished reports and data, and the review of data bases containing more than 7,000 analyses of ground-water samples for arsenic. In the first two environments, arsenic appears to be associated with sediments derived, in part, from volcanic rocks of intermediate to acidic composition. Dissolved arsenic concentrations in water from volcanic aquifers in the same regions, however, may be low (less than 10 micrograms per liter). Solid phases (minerals, amorphous solids, and sedimentary organic matter) that supply the dissolved arsenic have not been identified in most areas. Alluvial and lacustrine sedimentary deposits appear to be an important source of arsenic in volcanic areas (such as Lane County, Oregon) and in areas underlain by basin-fill deposits (such as Carson Desert in Nevada and the Tulare Lake basin in California). Mobilization of arsenic in sedimentary aquifers may be, in part, a result of changes in the geochemical environment due to agricultural irrigation. In the deeper subsurface, elevated arsenic concentrations are associated with compaction caused by groundwater withdrawals.