Perfluoroalkyl compounds (PFCs) were determined in 2 L surface water samples collected in the Atlantic Ocean onboard the research vessels Maria S. Merian along the longitudinal gradient from Las Palmas (Spain) to St. Johns (Canada) (15° W to 52° W) and Polarstern along the latitudinal gradient from the Bay of Biscay to the South Atlantic Ocean (46° N to 26° S) in spring and fall 2007, respectively. After filtration the dissolved and particulate phases were extracted separately, and PFC concentrations were determined using high-performance liquid chromatography interfaced to tandem mass spectrometry. No PFCs were detected in the particulate phase. This study provides the first concentration data of perfluorooctanesulfona-mide (FOSA), perfluorohexanoic acid, and perfluoroheptanoic acid from the Atlantic Ocean. Results indicate that trans-Atlantic Ocean currents caused the decreasing concentration gradient from the Bay of Biscay to the South Atlantic Ocean and the concentration drop-off close to the Labrador Sea. Maximum concentrations were found for FOSA, perfluorooctanesulfonate, and perfluorooctanoic acid at 302, 291, and 229 pg L ^-1, respectively. However, the concentration of each single compound was usually in the tens of picograms per liter range. South of the equator only FOSA and below 4° S no PFCs could be detected.