Assimilation of mercury (Hg) by vegetation represents one of the largest global environmental Hg mass fluxes. We estimate Hg assimilation by vegetation globally via a bottom-up scaling approach using tissue Hg concentrations synthesized from a comprehensive database multiplied by respective annual biomass production (NPP). As global annual NPP is close to annual vegetation die-off, Hg mass associated with global NPP approximates the transfer of Hg from plants to soils, which represents an estimate of vegetation-mediated atmospheric deposition. Annual vegetation assimilation of Hg from combined atmospheric and soil uptake is estimated at 3062 ± 607 Mg yr–1, which is composed of 2491 ± 551 Mg yr–1 from aboveground tissue uptake and 571 ± 253 Mg yr–1 from root uptake. Assimilation of atmospheric Hg amounts to 2422 ± 483 Mg yr–1 when considering aboveground tissues only. Atmospheric assimilation increases to 2705 ± 504 Mg yr–1 when considering that root Hg may be partially derived from prior foliar uptake and transported internally to roots. Estimated atmospheric Hg assimilation by vegetation is 54–137% larger than the current model and litterfall estimates, largely because of the inclusion of lichens, mosses, and woody tissues in deposition and all global biomes. Belowground, about 50% of root Hg was taken up from soils with currently unknown ecological and biogeochemical consequences.