The objectives of this work are to track the contamination levels, distribution characteristics, and sources of polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) in atmospheric particulate matter (APM) of Northern China and to provide more comprehensive and fundamental data for risk assessment of organochlorine contaminants (OCs) in environments. Samples were extracted and purified by the microwave-assisted extraction and solid-phase extraction system, respectively. PCBs and OCPs were analyzed by gas chromatograph-mass spectrometer. The concentrations of ΣPCBs and ΣOCPs ranged from 0.73 to 112.65 ng/g and 0.14 to 34.73 ng/g, respectively. PCBs in atmospheric particulates collected from Shijiazhuang City had the highest concentration, whereas OCP congeners were at the relatively low levels. However, the highest concentration of OCPs occurred in Yongning City. The principal component analysis indicated that the predominant compositions of PCBs in most of samples were tetrachlorobiphenyl (Tetra-CB), pentachlorobiphenyl (Penta-CB), hexachlorobiphenyl (Hexa-CB), and heptachlorbiphenyl (Hepta-CB), while hexachlorocyclohexanes (HCHs), DDTs, chlordanes, and endosulfans were the dominant components of OCPs, which was attributed to their application characteristics. OCs in those particles were further used to assess a potential cancer risk to humans via ingestion, dermal contact, and inhalation. Cancer risk was evaluated in airborne particles caused by PCBs and OCPs. TEQPCBs values suggested that the representative areas were subject to different pollution degrees. However, the pollution of OCPs in certain areas should be a concern due to 41.6% of the high risk, which could pose a potential risk to organisms.