This article provides a description of the processes used in modern aluminum reduction plants and explores the sources of polycyclic aromatic hydrocarbons (PAHs) at pertinent steps in the industrial process. Chemical and physical characteristics of raw and processed source materials are described, and the effects of process modifications and alternative processes on generation of PAHs are explored. For example, the self-bake Söderberg method is contrasted with the prebake method of anode formation by describing the quantities of PAHs generated and characteristics of PAHs associated with each process. Available datasets for aluminum smelters are predominantly limited to analyses of selected parent PAHs (unsubstituted). Thus, many preferred forensic methods for characterizing PAHs cannot be applied to much of the existing data. However, typical parent PAH distributions and isomer ratios are explored using up to 17 selected unsubstituted PAHs in emissions from aluminum reduction plants and environmental media affected by emissions. In addition, summaries are presented of selected environmental studies conducted in areas influenced by aluminum reduction and non-aluminum reduction sources of PAHs. Forensic tools for identifying influences from aluminum smelters in environmental samples reflecting mixed sources are also discussed.