In remote marine areas, biogenic productivity and atmospheric particulate are coupled through dimethylsulfide (DMS) emission by phytoplankton. Once in the atmosphere, the gaseous DMS is oxidized to produce H2SO4 and methanesulfonic acid (MSA); both species can affect the formation of cloud condensation nuclei. This study analyses eight years of biogenic aerosol evolution and variability at two Arctic sites: Thule (76.5° N, 68.8° W) and Ny Ålesund (78.9° N, 11.9° E). Sea ice plays a key role in determining the MSA concentration in polar regions. At the beginning of the melting season, in April, up to June, the biogenic aerosol concentration appears inversely correlated with sea ice extent and area, and positively correlated with the extent of the ice-free area in the marginal ice zone (IF-MIZ). The upper ocean stratification induced by sea ice melting might have a role in these correlations, since the springtime formation of this surface layer regulates the accumulation of phytoplankton and nutrients, allowing the DMS to escape from the sea to the atmosphere. The multiyear analysis reveals a progressive decrease in MSA concentration in May at Thule and an increase in July August at Ny Ålesund. Therefore, while the MSA seasonal evolution is mainly related with the sea ice retreat in April, May, and June, the IF-MIZ extent appears as the main factor affecting the longer-term behavior of MSA.