<jats:p>Abstract. Dimethyl sulfide (DMS) plays an important role in the atmosphere by influencing the formation of aerosols and cloud condensation nuclei. In contrast, the role of methanethiol (MeSH) for the budget and flux of reduced sulfur remains poorly understood. In the present study, we quantified DMS and MeSH together with the trace gases carbon monoxide (CO), isoprene, acetone, acetaldehyde and acetonitrile in North Atlantic and Arctic Ocean surface waters, covering a transect from 57.2 to 80.9∘ N in high spatial resolution in May–June 2015. Whereas isoprene, acetone, acetaldehyde and acetonitrile concentrations decreased northwards, CO, DMS and MeSH retained substantial concentrations at high latitudes, indicating specific sources in polar waters. DMS was the only compound with a higher average concentration in polar (31.2 ± 9.3 nM) than in Atlantic waters (13.5 ± 2 nM), presumably due to DMS originating from sea ice. At eight sea-ice stations north of 80∘ N, in the diatom-dominated marginal ice zone, DMS and chlorophyll a markedly correlated (R2 = 0.93) between 0–50 m depth. In contrast to previous studies, MeSH and DMS did not co-vary, indicating decoupled processes of production and conversion. The contribution of MeSH to the sulfur budget (represented by DMS + MeSH) was on average 20 % (and up to 50 %) higher than previously observed in the Atlantic and Pacific oceans, suggesting MeSH as an important source of sulfur possibly emitted to the atmosphere. The potential importance of MeSH was underlined by several correlations with bacterial taxa, including typical phytoplankton associates from the Rhodobacteraceae and Flavobacteriaceae families. Furthermore, the correlation of isoprene and chlorophyll a with Alcanivorax indicated a specific relationship with isoprene-producing phytoplankton. Overall, the demonstrated latitudinal and vertical patterns contribute to understanding how concentrations of central marine trace gases are linked with chemical and biological dynamics across oceanic waters. </jats:p>