Bulk atmospheric deposition of major cations (Na, K, Ca, Mg) and anions (Cl, F, SO 4 ) were measured at 15 sites around an active volcano, Mount Etna, from 2001 to 2003. Their composition indicates several natural sources, among which deposition of plume-derived volcanogenic gas compounds is prevalent for F, Cl and S. Plume-derived acidic compounds are also responsible for the prevailing acidic composition of the samples collected on the summit of the volcano (pH in the 2.45-5.57 range). Cation species have complex origin, including deposition of plume volcanogenic ash and aerosols and soil-dust wind re-suspension of either volcanic or carbonate sedimentary rocks.Variation of the deposition rates during the March 2001-March 2003 period, coupled with previous measurements from 1997 to (Appl Geochem 16:985-1000, were compared with the variation of SO 2 flux, volcanic activity and rainfall. The deposition rate was mainly controlled by rainfall. Commonly, about 0.1-0.9% of HF, HCl and SO 2 emitted by the summit crater's plume were deposited around the volcano. We estimate that ∼2 Gg of volcanogenic sulphur were deposited over the Etnean area during the 2002-2003 flank eruption, at an average rate of ∼24 Mg day −1 which is two orders of magnitude higher than that typical of quiescent degassing phases.