Concentrations of 119 pharmaceuticals and personal care products (PPCPs) and 13 perfluoroalkyl substances (PFASs) in marine sediments measured throughout Puget Sound (n = 10) and Bellingham Bay (n = 30), Washington, USA, are reported. These data are among the first measurements of PPCPs and PFASs in marine sediments from the Pacific Northwest and provide a comparison to previous measurements of these chemicals in influent, effluent, and biosolids from municipal wastewater treatment plants throughout the region. The concentrations of both PPCPs and PFASs in sediments from Puget Sound and Bellingham Bay ranged from very low to non-detectable for most compounds. Only 14 of the 119 PPCPs and 3 of 13 PFASs were quantifiable in sediments. Diphenhydramine (an antihistamine) was most frequently detected (87.5% of samples), with a maximum concentration of 4.81 ng/g dry weight and an estimated mean detected concentration of 1.68 ng/g. Triclocarban (an antibacterial) was detected in 35.0% of the samples, with a maximum concentration of 16.6 ng/g dry weight. Perfluoroalkyl substances were detected in 2.5% of analyses. Perfluorobutanoate, perfluorooctane sulfonate, and perfluorooctane sulfonamide were detected in 7, 5, and 1 sample(s) each, respectively, with the highest concentrations observed for perfluorooctane sulfonate (1.5 ng/g). Detected concentrations were often highest within the industrial harbor in Bellingham Bay and near the cities of Seattle and Bremerton. Environ Toxicol Chem 2013;32:1701-1710. © 2013 SETAC.