Carcinogenic polycyclic aromatic hydrocarbons (PAHs) are primarily released unintentionally. Exposure to PAHs is linked to increased cancer incidences. Here, we present a fully updated global emissions inventory of 30 parent PAHs from 1960 to 2021. With the availability of recently emerged important data sources, substantial improvements are achievable. Among the 147 sources quantified, over 90% originate from fewer than 10 major sources, particularly in the residential and industrial sectors. The temporal trend of emissions exhibits an inverse-U shape, positively influenced by energy consumption, population growth, and the production of coke, metals, and others, while negatively affected by energy transition, the phasing out of outdated production capacities, and end-of-pipe mitigation. Nonpriority dibenzopyrenes significantly contribute to overall toxicity. A notable correlation between BaP equivalent carcinogenicity (BaPeq) and all compounds, including benzo(a)pyrene (BaP), was revealed; BaP can represent the PAH mixture for toxicity from a global perspective, but care should be taken for different regions due to significant variations in source patterns and congener profiles.