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Per and polyfluoroalkyl substances (PFASs) have raised great concern due to their ubiquity in aquatic environments, and adsorption technologies are among the most promising treatment solutions. This study investigated the key factors that influence the adsorption of anionic PFASs on conventional and emerging adsorbents. Batch adsorption experiments were conducted to evaluate the removal of 20 target PFASs at environmentally relevant concentrations by three different activated carbon (AC) materials and two different β-cyclodextrin polymers (CDPs). Experiments were conducted in Milli-Q water and in groundwater. Major physical properties of the adsorbents were measured, along with general water chemistry parameters for each groundwater sample. Principal component analysis (PCA) was subsequently employed to extract the important associations from the multivariate dataset. The distinct performances of ACs and CDPs were attributed to their different surface chemistry and the distinct nature of their adsorption binding sites. Hydrophobic interactions dominated PFAS adsorption onto ACs while CDPs mostly attracted anionic PFASs via favorable electrostatic interactions. ACs of a smaller average particle size performed better, with our data pointing to an increased external specific surface area as the likely reason. pH and the concentration of cations were the primary contributors to adsorption inhibition in groundwater. Higher pH values limit anionic PFAS adsorption by deprotonating the functional groups on adsorbent surfaces. The elevated levels of cations in some groundwater samples limited the effects of attractive electrostatic interactions. Knowledge of PFAS adsorption mechanisms gained from this study can be used to design more efficient adsorbents and to predict their performance under a range of environmental scenarios., Competing Interests: Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Cornell University has filed US and international patent applications related to the porous cyclodextrin polymer studied in this manuscript. W.R.D. and D.E.H. serve on the scientific advisory board and have equity and/or stock purchase options in CycloPure, Inc., which is commercializing related porous cyclodextrin polymers and partially funded this study., (Copyright © 2020 Elsevier Ltd. All rights reserved.)