AbstractPesticides have adverse effects on human health and the environment and can be transported through the atmosphere from application sites and deposited to sensitive ecosystems. This study applies a comprehensive multimedia regional pesticide fate and chemical transport modeling system that we developed to investigate the atmospheric transport and deposition of toxaphene to the Great Lakes. Simulated results predict a significant amount of toxaphene (~350 kg) being transported through the atmosphere and deposited into the Great Lakes in the simulation year. Results also show that U.S. residues and global background are major sources to toxaphene deposition into the Great Lakes and atmospheric concentrations in the region. While the U.S. residues are the dominant source in warm months, the background dominates during winter months. In addition, different sources have different influences on the individual Great Lakes due to their proximity and relative geographical positions to the sources; U.S. residues are the dominant source to Lakes Ontario, Erie, Huron, and Michigan, but they are a much less important source to Lake Superior. These results shed light on the mystery that observed toxaphene concentrations in Great Lakes' lake trout and smelt declined between 1982 and 1992 in four of the Great Lakes except Lake Superior. While monthly total depositions to Lakes Ontario, Erie, Huron, and Michigan have clear seasonal variability with much greater values in April, May, and June, monthly total depositions to Lake Superior are more uniformly distributed over the year with comparatively greater levels in cold months.