Many studies have shown that atmospheric particulate-bound polycyclic aromatic hydrocarbons (AP-PAHs) pose carcinogenic and noncarcinogenic risks to human health. However, few studies have investigated the health risks of AP-PAHs across regional or national cities. Therefore, in this literature review, >6971 individual atmospheric samples from 89 cities in seven regions of China were obtained. The PAH contents in these samples were measured in accordance with national standards (HJ 784, 2016). AP-PAH contents (0.5–1.2 × 103 ng/m3) significantly increased in Chinese cities during 2002–2017. The contamination levels based on toxic equivalent quantities (0.6–1.4 × 102 ng/m3) were lower in the four southern regions than in the three northern regions. The health risks associated with AP-PAH exposure in different age group followed the following order: infants < kindergarten students < primary school students < middle school students < adults. This study revealed that AP-PAHs pose potential ecological risks and have adverse biological effects, and the mean effect range median quotient in 73 cities (82.0% of 89 cities) indicated moderate or high risk. Clustering analysis revealed that the primary sources of AP-PAHs are coal, petroleum, and biomass combustion. These results can be used to achieve AP-PAH pollution control in Chinese cities and worldwide.