Mollusk samples such as bivalves and gastropods were collected from eight sampling sites along Bohai Sea coastline from northeastern China. The samples were analyzed for polychlorinated biphenyls (PCBs), polychlorinated dibenzo-p-dioxins (PCDDs), and polychlorinated dibenzofurans (PCDFs) by high-resolution gas chromatography/high-resolution mass spectrometry (HRGC-HRMS) to elucidate bioaccumulation of persistent organic pollutants in benthon. Residue levels of ΣPCBs and ΣPCDD/Fs were in the ranges of 66.1 to 583.6 ng/g and 0.9 to 15317 pg/g on a lipid-weight basis, respectively, The pollution source was identified using principal component analysis (PCA) in some coastal areas. It indicated that the typical pollution sources were characterized by PCB3, which was one Chinese technical product of PCBs. PCA also revealed the similarity patterns of PCBs between identical species collected from the different sites. The higher gastropod PCB concentrations were related to a former capacitor factory and the paint factories in some coastal areas, but this was not the case with the bivalves. The results of this study suggest that some gastropod species may be a potential bioindicator or “sentinel” organism for marine PCBs monitoring.