Concentrations and species of iodine isotopes (127I and 129I) provide vital information about iodine geochemistry, environmental conditions and water masses exchange in oceans. Despite extensive investigations of anthropogenic 129I in the Arctic Ocean and the Nordic Seas, concentrations of the isotope in the Atlantic Ocean are, however, still unknown. We here present first data on 129I and 127I, and their species (iodide and iodate) in surface water transect along the northeastern Atlantic between 30° and 50°N. The results show iodate as the predominant species in the analyzed marine waters for both 127I and 129I. Despite the rather constant ratios of 127I−/127IO3−, the 129I−/129IO3− values reveal variations that apparently response to sources, environmental conditions and residence time. These findings provide a new tracer approach that will strongly enhance the application of anthropogenic 129I in ocean environments and impact on climate at the ocean boundary layer.