Mercury (Hg) is a persistent environmental contaminant and can accumulate and concentrate in food webs as methylmercury (MeHg), presenting a health risk to humans and wildlife. Multiyear monitoring and modeling studies have shown that atmospheric Hg in litterfall is an important form of Hg deposition to forests. Annual litterfall consists primarily of leaves with some amounts of needles, twigs, bark, flowers, seeds, fruits, and nuts. Atmospheric Hg accumulates in leaves and reaches an annual maximum concentration at autumn leaf drop. This data set is derived from autumn litterfall collected at 30 selected National Atmospheric Deposition Program (NADP) Mercury Deposition Network (MDN) sites in deciduous and mixed deciduous-coniferous forests from 16 states in the eastern United States during 2007-2009 and 2012-2015. The NADP administered litterfall collection at the MDN sites. The U.S. Geological Survey (USGS) distributed sets of passive litterfall sample collectors to MDN site operators for systematic retrieval of samples during the 8 to 16 weeks of autumn leaf drop each year at each site. Samples were processed and analyzed at the USGS Mercury Research Laboratory where concentrations of Hg and MeHg and litterfall dry mass and sample moisture were determined. All sites did not have data for all years. Most sites had four Hg concentrations per year and a few sites had less than or more than four Hg concentrations in specific years. MeHg concentrations were determined in one composite sample per site in 2007 and 2012-2015. Litterfall mass was determined from 4 to 8 samples per site per year. Seven annual groups of data were compiled into this dataset. More information is available from the NADP at http://nadp.sws.uiuc.edu/