Concentrations of mercury in the environment are increasing as a result of human activities, notably fossil-fuel burning and incineration of municipal wastes. Increasing levels of mercury in aquatic environments and consequently in fish populations are recognized as a public-health problem Enhanced mercury concentrations in lake sediments relative to pre-industrial values have also been attributed to anthropogenic pollution. It is generally assumed that atmospheric mercury deposition is dominated by global-scale processes, consequently being regionally uniform. Here, to the contrary, we report a significant gradient in concentrations and total amounts of mercury in organic litter and surface mineral soil along a transect of forested sites across the north central United States from northwestern Minnesota to eastern Michigan. This gradient is accompanied by parallel changes in wet sulphate deposition and human activity along the transect, suggesting that the regional variation in mercury content is due to deposition of anthropogenic mercury, most probably in particulate form.