Contamination of snow cover has been investigated in the Longyearbyen (78°13 N, 15°38 E) and Barentsburg (78°3 N, 14°12 E) areas, which are situated in the southwest part of Spitsbergen (Svalbard archipelago). Snow cover was sampled in two winter seasons, 2012–2013 and 2013–2014, at 54 locations within potentially contaminated areas. Sampling incorporated the whole snow mass and was combined with morphological observations as well as thickness and density measurements. Meltwater and suspended solids were further analysed for a wide range of contaminants including polycyclic aromatic hydrocarbons (PAHs) and macro-ions. Results were contrasted with previous studies measuring the release of contaminants from snow to soil cover. It was shown in keeping with earlier studies that PAH contributions are associated with airborne particulate matter. The results, in contrast to earlier studies further demonstrated that the high concentrations of contaminants in both settlements are attributed to local sources due to combustion and industrial activity.