Mercury (Hg) in autumn litterfall from predominately deciduous forests was measured in 3 years of samples from 23 Mercury Deposition Network sites in 15 states across the eastern USA. Annual litterfall Hg dry deposition was significantly higher (median 12.3 micrograms per square meter (μg/m(2)), range 3.5-23.4 μg/m(2)) than annual Hg wet deposition (median 9.6 μg/m(2), range 4.4-19.7 μg/m(2)). The mean ratio of dry to wet Hg deposition was 1.3-1. The sum of dry and wet Hg deposition averaged 21 μg/m(2) per year and 55% was litterfall dry deposition. Methylmercury was a median 0.8% of Hg in litterfall and ranged from 0.6 to 1.5%. Annual litterfall Hg and wet Hg deposition rates differed significantly and were weakly correlated. Litterfall Hg dry deposition differed among forest-cover types. This study demonstrated how annual litterfall Hg dry deposition rates approximate the lower bound of annual Hg dry fluxes.