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Abstract Bioaccessibility of particle-bound hydrophobic organic contaminants and related particle size effects are significant for assessing the potential human health risk via inhalation exposure, but have not been clearly evaluated. To fill this knowledge gap, the present study developed an in vitro method to estimate the inhalation bioaccessibility of particulate polycyclic aromatic hydrocarbons (PAHs) using simulated human lung fluids, i.e. , a modified Gamble's solution (MGS) and artificial lysosomal fluid (ALF) with Tenax as the absorption media. Assay parameters, namely incubation time (10 d) and influence of filter use, were optimized for establishing the in vitro method. The results showed that the bioaccessibility of PAHs increased with increasing particle size, but other factors, such as total organic carbon and chemical hydrophobicity, also played a large role in the fate of these compounds. The results from this portion of the present study were then used to evaluate human health risk, which showed that the risk of these particle-bound PAHs by incorporating size-dependent PAHs bioaccessibility and deposition efficiency in the human respiratory tract into inhalation exposure risk calculations was reduced by >90% when compared to using total concentration. This suggested that the inhalation bioaccessibility and deposition efficiency of hydrophobic organic chemicals should be included in human health risk assessment. Graphical abstract Unlabelled Image Highlights • An in vitro method was developed for evaluating the IBAF of particle-bound HOCs. • The inhalation bioaccessibility of PAHs decreased with increasing hydrophobicity. • The IBAF of particle-bound HOCs is significant to human health risk assessment. [ABSTRACT FROM AUTHOR]