The Vinto Sb-Sn smelter (Oruro, Bolivia) has been linked to arsenic and heavy metal pollution in air, soils, residual waters of the smelter, and hair and urine of workers, but crop concentrations had not been assessed previously. In this article, alfalfa, onions, and carrots, separated into roots and shoots, were analyzed for As and Pb, together with corresponding soil samples. The aim was to assess the environmental distribution and potential health impacts of these toxic elements and to compare them to levels observed at other sites around the world. As and Pb concentrations in all analyzed crop samples exceed the FAO/WHO, UK or Chilean limits by 1.5-2 orders of magnitude and As health risk indices were 286 (carrot) and 651 (onion), showing that the potential health risk due to consumption of these products is extremely high. As and Pb soil-plant transfer factors are similar to other contaminated sites around the world, but daily intake and health risk index for As are much higher in Vinto area due to very high concentrations in soils. Arsenic and lead soil and crop concentrations suggest increasing trends toward VMC. Correlations are significant for Pb in some crop fractions, but not for As, possibly due to considerable geogenic contributions to soil As in the area. In future surveys, larger numbers of soil and crop samples should be analyzed, and additional analyses should be carried out to distinguish anthropogenic and geogenic sources of As and Pb in soils and crops in the area.