Per- and poly-fluoroalkyl substances (PFASs) are man-made chemicals that are toxic and widely detected in the environment, including drinking water sources. A cost-effective treatment process for PFASs is currently not available. We developed reusable hydrogel sorbents to remove long- and short-chain perfluoroalkyl acids and 2,3,3,3-tetrafluoro-2-(heptafluoropropoxy)propanoic acid (GenX), which is are emerging PFAS. Through fluoridation and amination of poly(ethylene glycol) diacrylate (PEGDA), the newly synthesized sorbents can sorb the five targeted PFASs (perfluorooctanoic acid (PFOA), perfluorooctanesulfonic acid (PFOS), perfluorobutanesulfonic acid (PFBS), and perfluorobutanoic acid (PFBA) and GenX) to different degrees from aqueous solution. Aminated PEGDA showed the highest sorption capacity for all five PFASs, particularly for PFBA and PFBS. The bifunctionalized PEGDA showed higher capacities for PFOA and PFOS, suggesting that both hydrophobic interactions and charges contribute to the sorption. Both aminated and bifunctionalized sorbents can remove GenX from water, with the highest sorption capacity of 98.7 μmol g aminated PEGDA-1 within 6 h. The absorbed PFASs on the sorbents were observed and characterized by Fourier-transform infrared spectroscopy. The spent sorbents were reusable after readily regenerated with 70% methanol contained 1% NaCl.