The Of/Oh-horizons of 447 forest stands in Germany were evaluated for concentrations and spatial distribution of selected polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs), and organochlorine pesticides (OCPs). While concentrations of dichlorodiphenyltrichloroethane (DDT) and PCBs show similar spatial distribution patterns for all measured compounds within each compound class, significantly different distributions were identified for concentrations of low-molecular-weight PAHs [2- and 3-ring PAHs plus fluoranthene (FLA) and pyrene (PYR)] in contrast to high-molecular-weight PAHs (4-6-ring PAHs without FLA and PYR). Maxima of persistent organic pollutant (POP) concentrations could be mostly explained by specific locatable sources. Because of the slow degradation rates of these target substances, this is especially relevant for historic contamination sources, such as extensive 1980s DDT usage in the former German Democratic Republic and industrial facilities that produced hexachlorobenzene (HCB) or PCBs. A contribution of ubiquitous background pollution derived from long-range atmospheric transport is likely for some compounds in the studied area, e.g., DDT in the western part of Germany and dieldrin. However, most target compounds appear to be mainly sourced from local or regional emissions. This is supported by the absence of clear dependencies between POP concentrations and most evaluated environmental and local parameters. We suggest that these results generally reflect the distribution of POPs in densely populated and industrialized countries located in temperate regions.