Positive Matrix Factorization (PMF) was used to identify and apportion candidate sources of polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/F) in samples of offshore and coastal surface sediments from the Baltic Sea. Atmospheric deposition was the dominant source in offshore and pristine areas, in agreement with previous studies. Earlier chlorophenol use and a source suggested origins from pulp and paper production and related industries were identified as important coastal sources. A previously presumed major source, chlorine bleaching of pulp, was of only minor importance for modern Baltic surface sediments. The coastal source impacts were mostly local or regional, but pattern variations in offshore samples indicate that coastal sources may have some importance for offshore areas. Differences between sub-basins also indicated that local and regional air emissions from incineration or other high-temperature processes are more important in the southern Baltic Sea compared to those in northerly areas. These regional differences demonstrated the importance of including offshore sediments from the Bothnian Bay, Gulf of Finland, and other areas of the Baltic Sea in future studies to better identify the major PCDD/F sources to the Baltic Sea.