The relative importance of the Chicago/Gay urban area was investigated to determine its impact on atmospheric mercury (Hg) concentrations and wet deposition in the Lake Michigan basin. Event wet-only precipitation, total particulate, and vapor phase samples were collected for Hg, and trace element determinations from five sites around Lake Michigan from July 1994 through October 1995 as part of the Lake Michigan Mass Balance Study (LMMBS). In addition, intensive over-water measurements were conducted aboard the EPA research vessel Lake Guardian during the summer of 1994 and the winter of 1995 as part of the Atmospheric Exchange Over Lakes and Oceans Study. Atmospheric Hg concentrations were found to be significantly higher in the Chicago/Gary urban area than surrounding sites: Hg in precipitation was a factor of 2 and particulate Hg was a factor of 6 times higher. Overwater measurements found elevated Hg concentrations 19 km off shore of Chicago/Gary suggesting an enhanced near field atmospheric deposition to Lake Michigan. Meteorological transport analyses also determined that local sources in the Chicago/Gary urban area significantly impacted all of the LMMBS sites indicating a broad impact to the entire Lake Michigan basin.