A special version of the NOAA HYSPLIT_4 model has been developed and used to estimate the atmospheric fate and transport of mercury in a North American modeling domain. Spatial and chemical interpolation procedures were used to expand the modeling results and provide estimates of the contribution of each source in a 1996 anthropogenic US/Canadian emissions inventory to atmospheric mercury deposition to the Great Lakes. While there are uncertainties in the emissions inventories and ambient data suitable for model evaluation are scarce, model results were found to be reasonably consistent with wet deposition measurements in the Great Lakes region and with independent measurement-based estimates of deposition to Lake Michigan. Sources up to 2000 km from the Great Lakes contributed significant amounts of mercury through atmospheric transport and deposition. While there were significant contributions from incineration and metallurgical sources, coal combustion was generally found to be the largest contributor to atmospheric mercury deposition to the Great Lakes.