Fluoropolymer coatings demonstrate excellent chemical resistance and durability; however, their inherently low surface energy compromises adhesion and structural cohesion, particularly when exposed to aggressive environments. This study presents a scalable interfacial engineering strategy to enhance coating performance by integrating functionalized ground tire rubber (fGTR) into poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP). Post-consumer GTR is transformed into high-performance fillers through self-initiated grafting from copolymerization of acrylic acid (AA) and methyl methacrylate (MMA) on GTR surface. By varying the AA:MMA ratio on the GTR surface, tunable grafted interphases can be obtained and correlated with coating interfacial properties. Spectroscopy, thermal analysis, microscopy, wetting analysis, and electrochemical measurements were employed to characterize the coatings. Overall, this approach establishes the first demonstration of surface-functionalized, radical-active GTR as an interface-tunable additive in thin-film fluoropolymer coatings, enabling a sustainable route to multifunctional, corrosion-resistant barrier systems.
