AbstractPolyfluoroalkyl and perfluoroalkyl substances (PFASs), in the forms of neutral polyfluoroalkyl substances in the gas phase of air and ionic perfluoroalkyl substances in the dissolved phase of surface water, were investigated during a sampling campaign in the Bohai Sea, Yellow Sea, and Yangtze River estuary in May 2012. In the gas phase, the concentrations of neutral ∑ PFASs were within the range of 76–551 pg/m3. Higher concentrations were observed in the South Yellow Sea. 8:2 fluorotelomer alcohol (FTOH) was the predominant compound as it accounted for 92%–95% of neutral ∑ PFASs in all air samples. Air mass backward trajectory analysis indicated that neutral ∑ PFASs came mainly from the coast of the Yellow Sea, including the Shandong, Jiangsu, and Zhejiang provinces of China, and the coastal region of South Korea. The fluxes of gas phase dry deposition were simulated for neutral PFASs, and neutral ∑ PFASs fluxes varied from 0.37 to 2.3 pg/m2/s. In the dissolved phase of the surface water, concentrations of ionic ∑ PFASs ranged from 1.6 to 118 ng/L, with the Bohai Sea exhibiting higher concentrations than both the Yellow Sea and the Yangtze River estuary. Perfluorooctanoic acid (PFOA) was the predominant compound accounting for 51%–90% of the ionic ∑ PFAS concentrations. Releases from industrial and domestic activities as well as the semiclosed geographical conditions increased the level of ionic ∑ PFASs in the Bohai Sea. The spatial distributions of perfluoroalkyl carboxylic acids (PFCAs) and perfluoroalkane sulfonic acids (PFSAs) were different significantly. The Laizhou Bay was the major source region of PFCAs and the Yangtze River estuary was the major source of PFSAs.