The deposition and transport of mercury (Hg) has been studied extensively in rural environments but is less understood in urbanized catchments, where elevated atmospheric Hg concentrations and impervious surfaces may efficiently deliver Hg to waterways in stormwater runoff. We determined the rate at which atmospheric Hg accumulates on windows, identified the importance of washoff in removing accumulated Hg, and measured atmospheric Hg concentrations to help understand the relationship between deposition and surface accumulation. The main study location was Toronto, Ontario. Similar samples were also collected from Austin, Texas for comparison of Hg accumulation between cities. Windows provided a good sampling surface because they are ubiquitous in urban environments and are easy to clean/blank allowing the assessment of contemporary Hg accumulation. Hg Accumulation rates were spatially variable ranging from 0.82 to 2.7 ng m-2 d-1 in Toronto and showed similar variability in Austin. The highest accumulation rate in Toronto was at the city center and was 5?? higher than the rural comparison site (0.58 ng m-2 d-1). The atmospheric total gaseous mercury (TGM) concentrations were less than 2?? higher between the rural and urban locations (1.7 ?? 0.3 and 2.7 ?? 1.1 ng m-3, respectively). The atmospheric particulate bound fraction (HgP), however, was more than 3?? higher between the rural and urban sites, which may have contributed to the higher urban Hg accumulation rates. Windows exposed to precipitation had 73 ?? 9% lower accumulation rates than windows sheltered from precipitation. Runoff collected from simulated rain events confirmed that most Hg accumulated on windows was easily removed and that most of the Hg in washoff was HgP. Our results indicate that the Hg flux from urban catchments will respond rapidly to changes in atmospheric concentrations due to the mobilization of the majority of the surface accumulated Hg during precipitation events. ?? 2008 Elsevier Ltd.