Dimethyl sulfide (DMS) plays a major role in the global sulfur cycle. In addition, its atmospheric oxidation products contribute to the formation and growth of atmospheric aerosol particles, thereby influencing cloud condensation nuclei (CCN) populations and thus cloud formation. The pristine summertime Arctic atmosphere is a CCN-limited regime, and is thus very susceptible to the influence of DMS. However, atmospheric DMS mixing ratios have only rarely been measured in the summertime Arctic. During July–August 2014, we conducted the first high time resolution (10 Hz) DMS mixing ratio measurements for the Eastern Canadian Archipelago and Baffin Bay as one component of the Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments (NETCARE). DMS mixing ratios ranged from below the detection limit of 4 to 1155 pptv (median 186 pptv). A set of transfer velocity parameterizations from the literature coupled with our atmospheric and coincident seawater DMS measurements yielded air-sea DMS flux estimates ranging from 0.02–12 μmol m−2 d−1, the first published for this region in summer. Airmass trajectory analysis using FLEXPART-WRF and chemical transport modeling using GEOS-Chem indicated that local sources (Lancaster Sound and Baffin Bay) were the dominant contributors to the DMS measured along the 21 day ship track, with episodic transport from the Hudson Bay System. After adjusting GEOS-Chem oceanic DMS values in the region to match measurements, GEOS-Chem reproduced the major features of the measured time series, but remained biased low overall (median 67 pptv). We investigated non-marine sources that might contribute to this bias, such as DMS emissions from lakes, biomass burning, melt ponds and coastal tundra. While the local marine sources of DMS dominated overall, our results suggest that non-local and possibly non-marine sources episodically contributed strongly to the observed summertime Arctic DMS mixing ratios.