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Recent studies have demonstrated that soils formed on pyroclastic ash deposits are much more common in the Mediterranean area than previously assumed. These soils are an important key to understanding past volcanic events and landscape evolution. Chronological information in soils of Quaternary volcanic events, however, remains still poorly understood in southern Italy. Using a multi-method forensic approach, we explore the origin and age of volcanic deposits (soils) in Sicily and Calabria. The geochemical signature of the soil was compared to the chemical fingerprint of the magmas of potential source areas of southern Italian volcanoes. The results indicate that the investigated soils on the Nebrodi (Sicily) and Sila (Calabria) mountains were both impacted by materials having a high-K calc-alkaline series volcanism. The Aeolian Islands (in particular Lipari and Vulcano) are the most likely source of origin, but contributions also from the Etna (particularly the Biancavilla ignimbrites and Plinian eruptions) occurred. Weathering and leaching processes, along with a potential contribution from the underlying non-volcanic bedrock, has altered the main chemical composition of soils, often precluding direct relation to potential source areas. Immobile elements and their ratios (e.g. the Nb/Y vs Zr/Ti plot) or trace elements (Co, Th) and rare earth elements (laser ablation ICP-MS analyses of glass particles, volcanic clasts and pumice-like materials) gave precious hints of the origin of the volcanic deposits. Radiocarbon dating of the H2O2 resistant soil organic fraction indicates a minimum age of 8–10 ka of the soils. The weathering index WIP (weathering index according to Parker) and the chemical composition of volcanic glasses and clasts were tested as proxies for the age of the volcanic deposits and time for soil formation. The soils and landscape are characterised by multiple volcanic depositional phases for the last about 50 ka in the Sila mountains and about 70 ka or more in the Nebrodi mountains. Chemical-mineralogical analyses enabled the detection of deposition phases during the Pleistocene and also Holocene. The multi-method approach enabled the identification of potential source areas, provided a tentative age estimate of the start (and in part duration) of ash deposits and therefore improved our understanding of volcanic landscape evolution.