Elevated levels of non-sea-salt sulfate and SO2 in samples collected off the west coast of South America indicate that there is a major source of atmospheric sulfur in the region of southern Peru and northern Chile. During a 1983 cruise, observed concentrations of non-sea-salt sulfur, SO2, selenium, arsenic, and antimony were comparable to levels reported for moderately polluted urban air. In contrast, methanesulfonic acid levels were typical of coastal marine air. Clearly, the elevated atmospheric sulfur levels in this region cannot be ascribed to oceanic organosulfur emissions. The major inputs are tentatively attributed to the smelting of sulfide ores which is a major industry in this region. The transport of smelter derived aerosols to this region may have a number of consequences for the atmospheric and oceanic chemistry of the Peruvian upwelling area.