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This work studied the contribution of the geogenic sources volcanoes and fumaroles to the aerosol in marine atmosphere in the central Mediterranean basin. For this purpose, in the framework of the Med-Oceanor measurement program, we carried out a cruise campaign in the summer of 2017 to investigate the impact to the aerosol of the most important Mediterranean volcanoes (Mount Etna, Stromboli Island, and Marsili Seamount) and solfatara areas (Phlegraean Fields complex, Volcano Islands, Ischia Island, and Panarea submarine fumarole). We collected PM10 and PM2.5 samples in 12 sites and performed chemical characterization to gather information about the concentration of major and trace elements, elemental carbon (EC), organic carbon (OC), and ionic species. The use of triangular plots and the calculation of enrichment factors confirmed the interception of volcanic plume. We integrated the outcomes from chemical characterization with the use of factor analysis and SEM/EDX analysis for the source apportionment. Anthropogenic and natural sources including shipping emissions, volcanic and fumarolic load, as well as sea spray were identified as the main factors affecting aerosol levels in the study area. Furthermore, we performed pattern recognition analysis by stepwise linear discriminant analysis to seek differences in the composition of PM10 and PM2.5 samples according to their volcanic or solfatara origin., This research was funded by the European Commission—H2020, the ERA-PLANET programme (www.era-planet.eu; contract no. 689443) within the IGOSP project (www.igosp.eu).