The urgent need for per- and polyfluoroalkyl substances (PFAS) remediation has driven research into innovative materials capable of efficient and sustainable removal. Poly(N-isopropylacrylamide) (PNIPAAm), a thermoresponsive polymer, presents a promising solution due to its tunable properties and potential for reversible sorption. In this study, PNIPAAm-based systems were developed and functionalized with cationic monomers such as diallyldimethylammonium chloride (DADMAC) and trimethylammonium chloride (DQ) to enhance PFAS binding. Additionally, styrene, a hydrophobic monomer, was incorporated to improve flocculation and decrease the lower critical solution temperature (LCST), making the flocculation process more energy-efficient and applicable to large-scale water treatment systems. The LCST was evaluated using UV-Vis spectroscopy. Liquid chromatography–mass spectrometry (LC-MS) was used to quantify PFAS removal and compare the relative affinities of different polymer systems. This work highlights the potential of functionalized smart polymers as a scalable, low-energy alternative for PFAS remediation in industrial applications.