The environmental distribution of per- and polyfluoroalkyl substances (PFAS) in water, snow, sediment and soil samples taken along the west coast of Spitsbergen in the Svalbard archipelago, Norwegian Arctic, was determined. The contribution of potential local primary sources (wastewater, firefighting training site at Svalbard airport, landfill) to PFAS concentrations and long-range transport (atmosphere, ocean currents) were then compared, based on measured PFAS levels and composition profiles. In remote coastal and inland areas of Spitsbergen, meltwater had the highest mean ΣPFAS concentration (6.5 ± 1.3 ng L−1), followed by surface snow (2.5 ± 1.7 ng L−1), freshwater (2.3 ± 1.1 ng L−1), seawater (1.05 ± 0.64 ng L−1), lake sediments (0.084 ± 0.038 ng g−1 dry weight (dw)) and marine sediments (−1 dw, median 0.015 ng g−1 dw). Perfluoroalkyl sulfonates (PFSA) and 6:2 fluorotelomer sulfonate (FTSA) were predominant in water and soil samples influenced by local sources, while perfluoroalkyl carboxylates (PFCA) were predominant in water and sediment from remote coastal and inland areas of Svalbard. The PFAS composition profiles observed in remote areas indicated that atmospheric transport and oxidation of volatile precursors is an important source of PFCA on Svalbard. Shorter-chain PFAS such as perfluorobutanoate (PFBA) were the predominant PFAS in freshwater, reflecting replacement of C8-chained PFAS with shorter-chained compounds. The comparatively high PFAS (especially PFBA) concentration in meltwater indicated that melting of snow and ice during the Arctic spring is an important diffuse local PFAS source. This source may become even more important with climate warming-induced melting of Arctic glaciers and ice sheets. Further studies of mobilisation and transport of PFAS in the Arctic region are needed to confirm this trend