Polycyclic aromatic hydrocarbons (PAHs) are the most highly concerned pollutants bound on traffic-impacted particulate matter (TIPM). The inhaled TIPM-bound PAHs risk has attracted much attention, whereas the inhalation bioaccessibility, a method to refine the exposure risk assessment, has not yet been extensively introduced in the exposure risk assessment. Thus, in vitro assays using artificial lung fluids including artificial lysosomal fluid (ALF), Gamble's solution (GS), and modified GS (MGS) were conducted to assess the inhalation bioaccessibility of USEPA 16 PAHs in TIPM collected from an expressway tunnel, the influence factors of PAHs' inhalation bioaccessibility were explored, and the exposure risk of TIPM-bound PAHs was estimated based on inhalation bioaccessibility. Results showed that the average PAHs concentrations were 30.5 ± 12.9 ng/m3, 36.2 ± 5.19 ng/m3, and 39.9 ± 4.31 ng/m3 in the tunnel inlet PM2.5, TSP, and tunnel center PM2.5, respectively. Phe, Flt, Pyr, Nap, Chr, BbF, and BkF were found as the dominant species in TSP and PM2.5, indicating a dominant contribution of PAHs from diesel-fueled vehicular emissions. The bioaccessible fractions measured for different PAH species in tunnel PM2.5 and TSP were highly variable, which can be attributed to PAHs' physicochemical properties, size, and carbonaceous materials of TIPM. The addition of Tenax into SLF as an “adsorption sink” can greatly increase PAHs' inhalation bioaccessibility, but DPPC has a limited effect on tunnel PM-bound PAHs' bioaccessibility. The incremental lifetime carcinogenic risk (ILCR) of tunnel inlet PM2.5-bound PAHs evaluated according to their total mass concentration exceeded the threshold (1.0 × 10−6) set by the USEPA, whereas the ILCRs estimated based on the inhalation bioaccessibility were far below the threshold. Hence, it is vitally important to take into consideration of pollutant's bioaccessibility to refine health risk assessment.