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Polycyclic aromatic compounds (PACs) in Canadian air and deposition were examined at the national scale for the first time in over twenty-five years. Air concentrations spanned four orders of magnitude, and were highest near industrial emitters and lowest in the Arctic. Declines in unsubstituted PAHs were observed at locations close to industrial facilities that had reduced emissions, but trends elsewhere were modest or negligible. Retene concentrations are increasing at several locations. Ambient concentrations of benzo[a]pyrene exceeded Ontario's health-based guideline in many urban/industrial areas. The estimated toxicity of the ambient PAC mixture increased by up to a factor of six when including compounds beyond the US EPA PAHs. Knowledge of PAC deposition is limited to the Laurentian Great Lakes and Athabasca Oil Sands regions. The atmosphere remained a net source of PAHs to the Great Lakes, though atmospheric inputs were decreasing with halving times of 26-30 years. Chemical transport modelling substantially overestimated wet deposition, but model performance is unknown for dry deposition. Sources from Asia, Europe and North America contributed to Arctic and Sub-Arctic concentrations, whereas transboundary or long-range transport have not been assessed outside Canada's north. Climate-related impacts from re-emission and forest fires were implicated in maintaining air concentrations in the high Arctic that were not consistent with global emissions reductions. Industrial emission decreases were substantial at the national scale, but their influence on the environment was limited to areas near relevant facilities. When examined through the lens of ambient levels at the local scale, evidence suggested that contributions from residential wood combustion and motor vehicles were smaller and larger, respectively, than those reported in national inventories. Future work aimed at characterizing PACs beyond the EPA PAHs, improving measurement coverage, elucidating deposition phenomena, and refining estimates of source contributions would assist in reducing remaining knowledge gaps about PACs in Canada., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Crown Copyright © 2020. Published by Elsevier Ltd. All rights reserved.)