Bioaccumulation of dissolved elemental mercury (DGM) by various organisms has been demonstrated, but no study has shown its uptake and sequestration by phytoplankton species. The present study aims to investigate the accumulation of mercury by phytoplankton species exposed to DGM. Diatoms (Cyclotella meneghiniana and Navicula pelliculosa) and green algae (Chlamydomonas reinhardtii and Haematococcus pluvialis) were exposed to constant high level of atmospheric gaseous Hg (∼7.7 µg m−3). Total mercury concentrations (THg) in the medium (dissolved fraction) and algae cells (cellular fraction) were determined using cold vapor atomic fluorescence spectroscopy. Results revealed a partitioning of Hg(0) between the atmosphere and phytoplankton cultures, with THg predominantly found in the algae cells. THg in the algae cultures decreased in the order: C. reinhardtii >H. pluvialis >N. pelliculosa >C. meneghiniana. However, the cellular concentration (mol cell−1) decreased in the order: H. pluvialis >C. reinhardtii >C. meneghiniana >N. pelliculosa. These results highlight species specificity in Hg accumulation upon exposure to DGM, further linked to the phytoplankton surface area. Our findings reveal for the first time that phytoplankton species significantly influence the partitioning of atmospheric Hg(0) in aquatic environments, with important implications for the understanding of the aquatic mercury cycle.