The American Smelting and Refining Company (ASARCO) smelter in Ruston, Washington, contaminated the south-central Puget Sound region with heavy metals, including arsenic and lead. Arsenic and lead distribution in surface sediments of 26 lakes is significantly correlated with atmospheric model predictions of contaminant deposition spatially, with concentrations reaching 208mg/kg As and 1375mg/kg Pb. The temporal distribution of these metals in sediment cores is consistent with the years of operation of the ASARCO smelter. In several lakes arsenic and lead levels are highest at the surface, suggesting ongoing inputs or redistribution of contaminants. Moreover, this study finds that arsenic is highly mobile in these urban lakes, with maximum dissolved arsenic concentrations proportional to surface sediment levels and reaching almost 90μg/L As. With 83% of the lakes in the deposition zone having surface sediments exceeding published “probable effects concentrations” for arsenic and lead, this study provides evidence for possible ongoing environmental health concerns.