As part of the Integrated Atmospheric Deposition Network (IADN), air samples were collected at five sites around the Great Lakes (two urban, two rural, and one remote) every 12 days during 2005-2006, and the concentrations of polybrominated diphenylethers (PBDEs), 1,2-bis(2,4,6-tribromophenoxy)-ethane (TBE), Dechlorane Plus (DP), and decabromodiphenyl ethane (DBD PE) were measured. The highest mean concentrations of total PBDEs were found at the urban sites in Chicago and Cleveland (65 +/- 4 and 87 +/- 8 pg/m3, respectively), and the lowest at the remote site in Eagle Harbor (5.8 +/- 0.4 pg/m3). With the exception of Chicago, the atmospheric concentrations of BDE-47 and 99 (summed over the gas and particle phases) are decreasing rapidly with half-lives of approximately 2 years, but the concentrations of BDE-209 are not decreasing at any of the five sites. The atmospheric partial pressures of BDE-47 and 99 showed a strong Clausius-Clapeyron relationship with reciprocal atmospheric temperature. TBE, DBDPE and DP were detected at all sites, but with the exception of Chicago, there were insufficient data to determine temporal trends for these compounds. The influence of human population density and synoptic atmospheric transport patterns was explored to explain the relatively high concentrations of BDE-209 in Cleveland.