Measurements of ocean surface and atmospheric dimethyl sulfide (DMS) and particle size distributions were made in the Canadian Arctic Archipelago during the fall of 2007 and the late summer of 2008 aboard the Canadian Coast Guard Ship Amundsen. Nucleation-mode particles were observed during the 2008 cruise, which took place in the eastern Arctic from August to September when the atmosphere and ocean were more photo-active as compared to the October 2007 transit in the Beaufort Sea during which no nucleation/growth events were observed. The observed nucleation periods in 2008 coincided with high atmospheric and ocean surface DMS concentrations, suggesting that the particles originated from marine biogenic sources. An aerosol microphysics box model was used to simulate nucleation given the measured conditions in the marine boundary layer. Although other sources may have contributed, we find that the newly formed particles can be accounted for by a marine biogenic DMS source for combinations of the following parameters: [OH] ≥ 3 × 105 molecules cm−3, DMS mixing ratio is ≥ 100 pptv, the activation coefficient is ≤ 10−7 and the background particle concentration is ≤ 100 cm−3.