Selective removal of persistent “forever chemicals” drives this collaborative research effort to develop a new class of bioinspired electrocatalytic platforms for per- and polyfluoroalkyl substance (PFAS) degradation, with initial focus on perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS). The work combines expertise in surface-confined redox-active materials and electrochemical remediation with the Korendovych group’s catalytic amyloid peptide nanostructures, which offer enzyme-like activity and tunable architectures. Short peptide libraries will be designed to self-assemble into catalytic amyloids capable of activating carbon–fluorine bonds under electrochemical conditions, enabling low-cost combinatorial synthesis and machine-learning-assisted discovery and optimization. Fluorinated peptide sequences will also be explored to create amyloid domains with enhanced fluorous-phase character, supporting selective PFAS adsorption through fluorophilic interactions and molecular recognition. Catalytic amyloids will be integrated into conductive electrode architectures via surface-immobilization and electrografting methods optimized for stability, redox mediation, and interfacial electron transfer. Electrochemical testing under environmentally relevant aqueous conditions will quantify degradation performance and defluorination while probing electron–proton transfer mechanisms. In situ spectroelectrochemical approaches, including electrochemical mass spectrometry and fluorine nuclear magnetic resonance (NMR), will track degradation pathways in real time to strengthen mechanistic understanding and guide iterative design.