Bulk atmospheric deposition of major cations (Na, K, Ca, Mg) and anions (Cl, F, SO4) 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 2000 (Appl Geochem 16:985-1000, 2001), were compared with the variation of SO2 flux, volcanic activity and rainfall. The deposition rate was mainly controlled by rainfall. Commonly, about 0.1-0.9% of HF, HCl and SO2 emitted by the summit crater's plume were deposited around the volcano. We estimate that similar to 2 Gg of volcanogenic sulphur were deposited over the Etnean area during the 2002-2003 flank eruption, at an average rate of similar to 24 Mg day(-1) which is two orders of magnitude higher than that typical of quiescent degassing phases.