In this study a large dataset on the polycyclic aromatic hydrocarbon (PAH) content of Swiss soils was analysed to evaluate two source apportionment tools, i.e., characteristic PAH ratios/molecular markers and a linear mixing model. Population density and total organic carbon (TOC) content were identified by a multiple regression model as independently and positively influencing the PAH concentrations in Swiss background soil. Specifically, TOC was more strongly positively correlated with the sum of light PAH (naphthalene to phenanthrene) than with the sum of heavy PAH (anthracene to benzo[ghj]perylene), whereas population density was more strongly positively correlated with the sum of heavy PAH than with light PAH. In addition, the sum of the heavy PAH as well as the total sum correlated negatively with sample site altitude. It is therefore hypothesised that heavy PAH are less mobile, whereas light PAH were closer to equilibrium with TOC in the soil. Similar results were found for polychlorinated biphenyls (PCB). The characteristic ratios and molecular markers pointed to pyrogenic origin of PAH in Swiss background soil but did not allow for further differentiation of individual fuel contributions, even though attempts to take environmental fractionation processes into account were made. The comparison of three soil profiles identified with a linear mixing model from the pattern of 16 PAH with >300 PAH emission profiles from the literature suggested urban dust, wood combustion and binders from asphalt as PAH sources. However, also here, environmental fractionation processes probably obscured source characteristic PAH ratios and fingerprints, which thus need to be interpreted with caution.