An oceanographic cruise campaign on-board the Italian research vessel Urania was carried out from the 26th of August to the 13th of September 2010 in the Eastern Mediterranean. The campaign sought to investigate the mercury cycle at coastal and offshore locations in different weather conditions. The experimental activity focused on measuring mercury speciation in both seawater and in air, and using meteorological parameters to estimate elemental mercury exchange at the sea–atmosphere interface. Dissolved gaseous mercury (DGM), unfiltered total mercury (UTHg) and filtered total mercury (FTHg) surface concentrations ranged from 16 to 114, 300 to 18,760, and 230 to 10,990pgL−1, respectively. The highest DGM, UTHg and FTHg values were observed close to Augusta (Sicily), a highly industrialized area of the Mediterranean region, while the lowest values were recorded at offshore stations. DGM vertical profiles partially followed the distribution of sunlight, as a result of the photoinduced transformations of elemental mercury in the surface layers of the water column. However, at some stations, we observed higher DGM concentrations in samples taken from the bottom of the water column, suggesting biological mercury production processes or the presence of tectonic activity. Moreover, two days of continuous measurement at one location demonstrated that surface DGM concentration is affected by solar radiation and atmospheric turbulence intensity. Atmospheric measurements of gaseous elemental mercury (GEM) showed an average concentration (1.6ngm−3) close to the background level for the northern hemisphere. For the first time this study used a numerical scheme based on a two-thin film model with a specific parameterization for mercury to estimate elemental mercury flux. The calculated average mercury flux during the entire cruise was 2.2±1.5ngm−2h−1. The analysis of flux data highlights the importance of the wind speed on the mercury evasion from sea surfaces. ► The Hg cycle in the East Mediterranean Marine Boundary Layer was examined. ► Sunlight, wind and CDOM influenced dissolved gaseous mercury. ► Anthropogenic influences on concentrations and fluxes were found to be important.