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Air and seawater samples were collected on board the R/V Polarstern during a scientific expedition from Germany to the Arctic Ocean during June–August 2004. The air data show a strong decline with latitude with the highest polychlorinated biphenyl (PCB) concentrations in Europe and the lowest in the Arctic. ΣICES PCBs in air range from 100 pg m−3 near Norway to 0.8 pg m−3 in the Arctic. A comparison with other data from previous and ongoing land‐based air measurements in the Arctic region suggests no clear temporal decline of PCBs in the European Arctic since the mid‐1990s. Dissolved concentrations of Σ6PCBs (28/31, 52, 101, 118, 138, 153) in surface seawater were L−1. Dominant PCBs in seawater were 28/31 and 52 (0.1–0.44 pg L−1), with PCBs 101, 118, and 138 < 0.1 pg L−1. In seawater, PCB 52 displayed the highest concentrations in the northernmost samples, while PCBs 101, 118, and 138 showed slightly decreasing trends with increasing latitude. Fractionation was observed for PCBs in seawater with the relative abundance of PCBs 28 and 52 increasing and that of the heavier congeners decreasing with latitude. However, in air only 15–20% of the variability of atmospheric PCBs can be explained by temperature. Owing to large uncertainties in the Henry's Law constant (HLC) values, fugacity quotients for PCBs were estimated using different HLCs reported in the literature. These indicate that on average, deposition dominates over volatilization for PCBs in the Arctic region with a strong increase in the middle of the transect near the marginal ice zone (78–79°N). The increase in fugacity ratio is mainly caused by an increase in air concentration in this region (possibly indirectly caused by ice melting being a source of PCBs to the atmosphere).