Turkish Government has officially become a party to the Stockholm Convention as of 2010, therefore, determination of POPs in environmental compartments in Turkey is a critical concern. In this study, 22 organochlorine pesticides (OCPs) and 43 polychlorinated biphenyls (PCBs) were measured in gas and particulate phases of ambient air samples collected in Izmir and Istanbul from May to October 2014 on a weekly basis. Gas chromatography–mass spectrometry was used to quantify the targeted pollutants. Potential source regions were assessed by applying back-trajectory and Potential Source Contribution Function (PSCF). Population carcinogenic risk levels associated with inhalation exposure were estimated by using Monte Carlo simulation, for which sensitivity and uncertainty analyses were also conducted. The highest mean concentration compounds were heptachlor (61±126 pg/m3) and p,p’-DDE (54±57 pg/m3) in Izmir and Istanbul, respectively. The mean Ʃ43PCBs concentration was found as 232±224 pg/m3 in Izmir, and 104±48 pg/m3 in Istanbul. Gas phase concentartions of OCPs and PCBs were generally much higher than particle phase. The PSCF results pointed out different potential source regions: Middle East, Eurasia, and Europe. All the estimated carcinogenic risks based on the 95% percentile values for individual OCPs and Ʃ43PCBs were calculated below the acceptable risk levels (10-6), indicating no significant potential health risk via inhalation route.