The concentrations of 23 polycyclic aromatic hydrocarbons (PAHs; 16 parent PAHs and 7 alkyl-PAHs) were determined in 45 surface sediment and 7 basal sediment box core samples retrieved from the Estuary and Gulf of St. Lawrence in eastern Canada. The concentration sums of 16 priority PAHs (Σ16PAHs) in the surface sediments (representing modern times or at least younger than the last decade) ranged from 71 to 5672 ng g−1. Σ16PAHs in the basal sediments ranged from 93 to 172 ng g−1 among the pre-industrial samples (pre-1900 common era or CE) and from 1216 to 1621 ng g−1 among the early post-industrial samples (~1930s and ~1940s CE). The highest Σ16PAH values occurred in samples retrieved from the Baie-Comeau-Matane area, an area affected by intense industrial anthropogenic activities. Source-diagnostic PAH ratios suggest a predominance of pyrogenic sources via atmospheric deposition, with a minor contribution of petrogenic seabed pockmark sources. The PAH concentrations in the sediments from the study areas reveal low ecological risks to benthic or other organisms living near the water-sediment interface.