High volume air samples taken onboard several research vessels in the Atlantic Ocean, the Southern Ocean, and the Baltic Sea as well as at one land-based site close to Hamburg, Germany, in 2007 and 2008 were analyzed for per- and polyfluorinated organic compounds (PFCs). A set of neutral, volatile PFCs such as fluorotelomer alcohols (FTOH) or perfluoroalkyl sulfonamides and ionic nonvolatile PFCs like perfluorinated carboxylates (PFCA) and sulfonates (PFSA) were collected on PUF/XAD-2/PUF cartridges and glass fiber filters and determined using GC-MS and HPLC-MS/MS. PFCs were detected in all air samples, even in Antarctic regions, and occurred predominantly in the gas phase. Total gas-phase concentrations of ship-based samples ranged from 4.5 pg m^-3 in the Southern Ocean to 335 pgm^-3 in European source regions. Concentrations of 8:2 FTOH, the analyte that was usually observed in highest concentrations, were between 1.8 and 130 pg m^-3. PFC concentrations decreased from continental regions toward marine regions and from Central Europe toward the Arctic and Antarctica. Southern hemispheric concentrations of individual PFCs were significantly lower than those of the northern hemisphere. On the basis of this data set, marine background PFC concentrations and atmospheric residence times were calculated. This study gives further evidence that volatile PFCs undergo atmospheric long-range transport to remote regions and may contribute to their contamination with persistent PFCA and PFSA.