Atmospheric polycyclic aromatic hydrocarbons (PAHs) are environmental pollutants that represent a risk not only to humans, but to all living organisms. High-molecular weight PAHs are more toxic than lighter relatives, and also have a higher tendency to bind onto air particles (i.e., particle matter, PM). PM is a major constituent of air pollution. Adequate assessment of the biological impact of PM requires the analysis, not only of the effects on human health, but also on the environment. Since the aquatic systems work as a natural sink to these air pollutants, assessing the effects of particle-bound PAHs on aquatic organisms may further characterize its potential aquatic toxicity, also providing simple and low-cost alternative assays to investigate PM biological effects in vivo. We review the current scientific literature, addressing the atmospheric PAHs fate, transformation and deposition, pertinent particle-bound PAHs toxicity data, and the potential aquatic toxic burden. Conceptual and experimental procedures that could improve future investigations and risk assessments are also considered.