Herein, we developed a β-cyclodextrin (β-CD)-based polymer crosslinked with tripodal amine to demonstrate the synergetic effects of the superior adsorption of both short- and long-chain per- and polyfluoroalkyl substances (PFASs). Kinetics studies showed rapid adsorption (~100% for nine PFASs at 1 µg L−1, except PFBA, and >86% at 200 µg L−1 individually) within 2 min. Isotherm results showed exceptional adsorption affinity and capacity, with K