As the concerns over the ubiquity and toxicity of per- and polyfluoroalkyl substances (PFASs) grow, research has focused on finding both technically and financially efficient PFAS remediation technologies. When evaluating certain technologies, research has focused on the removal of perfluoroalkyl acids from water, but contaminated groundwater often contains complex mixtures of diverse groups of PFASs. Utilizing a more comprehensive method to evaluate the performance of different PFAS treatment technologies involving the consideration of environmental matrix complexity can bring more useful insights into practical application. Adsorption-based processes are among the most promising technologies available for PFAS removal from water. The conventional adsorbents including activated carbon (AC) and anion exchange (AE) resins have been implemented in pilot or full-scale processes targeting PFAS removal from water. Emerging adsorbents, including novel β-cyclodextrin polymers (CDPs), have also exhibited potential for PFAS removal from water. The efficacy of CDPs on PFAS removal and the importance of varying surface properties of different CDPs on determining the affinity and selectivity to contaminants have been demonstrated. However, the mechanisms by which adsorbates bind to CDPs remains poorly understood. More research is needed to elucidate the mechanisms about the relative contributions of hydrophobic and electrostatic interactions for the adsorption of PFASs on CDPs.Two studies were designed to systematically explore the potential of conventional adsorbents and novel CDPs to remove mixtures of PFASs from contaminated groundwater and probe the adsorption binding mechanisms for anionic PFAS removal on CDPs. The first study aimed to evaluate the performance of five adsorbents including one AC, one AE resin and three different CDPs with varying surface charges to remove 68 PFASs in contaminated groundwater integrating a suspect screening approach. The PFAS removal performance of the adsorbents was evaluated with respect to adsorption affinity, kinetics, and selectivity. This evaluation provided insights on the factors that determine PFASs adsorption, which can be associated with the increasing length of the perfluorinated tail or could be more strongly related to properties of the head group. The second study aimed to evaluate the relative contributions of hydrophobic and electrostatic interactions on the adsorption of anionic PFASs by CDPs under controlled experimental conditions in nanopure water and different salt-amended nanopure water matrices. This study provided new insights into the adsorption binding mechanisms between anionic PFASs and CDPs as a function of chain length, and revealed the effects of different types and concentrations of inorganic constituents on the adsorption mechanisms. Together, the research described in this thesis furthers the understanding of different PFAS removal patterns by different adsorbents, and the understanding of anionic PFAS adsorption mechanisms on CDPs. These findings can serve as guidance and knowledge support on the future development and practical application of CDPs for different PFAS species under a range of environmental conditions.