Dimethylsulfide (DMS) atmospheric and oceanic concentrations and eddy covariance air/sea fluxes were measured over the N. Atlantic Ocean during July 2007 from Iceland to Woods Hole, MA, USA. Seawater DMS levels north of 55°N ranged from 3 to 17 nM, with variability related to the satellite-derived distributions of coccoliths and to a lesser extent, chlorophyll. For the most intense bloom region southwest of Iceland, DMS air/sea fluxes were as high as 300 μmol m−2 d−1, larger than current model estimates. The observations imply that gas exchange coefficients in this region are significantly greater than those estimated using most gas transfer parameterizations. South of 55°N, DMS levels were lower and the gas transfer coefficients were similar to those observed in other regions of the ocean. The data suggest that DMS emissions from the bloom region may be significantly larger than current estimates. The anomalous gas exchange coefficients likely reflect strong near-surface, water column DMS gradients influenced by physical and biological processes.