Atmospheric sources contributed significantly to the annual flux of trace metals and sulfate to the forest floor of Walker Branch Watershed, a forested catchment in the southeastern United States. Atmospheric deposition supplied from 14% (Mn) to≈40% (Zn, Cd, So4=) to 99% (Pb) of the annual flux to the forest floor; the remainder was attributable to internal element cycling. The measured water solubility of these metals in suspended and deposited particles indicates that they may be readily mobilized following deposition. Dry deposition constituted a major fraction of the total annual atmospheric input of Cd and Zn (≈20%), SO=(≈35%), Pb(≈55%), and Mn (≈90%); however, wet deposition rates for single events exceeded dry deposition rates by one to four orders of magnitude. Interception of rain by the canopy resulted in loss of Cd, Mn, Pb, Zn, and SO= from the canopy, but uptake of H+ which increased with increasing free acidity of the incoming rain, and with increasing residence time of the rain on the leaf surface.