Per- and polyfluoroalkyl substances (PFAS) present significant water contamination challenges due to their environmental persistence and health implications. This study evaluates the sustainability of granular activated carbon (GAC) and ion exchange (IX) remediation technologies through comprehensive cost and environmental impact assessments. System size emerges as a critical factor influencing sustainability outcomes through economies of scale and environmental trade-offs. Current cost estimation models like the EPA's Work Breakdown Structure approach lack sufficient uncertainty and sensitivity analyses, limiting their applicability across variable conditions. Our findings demonstrate that integrating life cycle assessment (LCA) with techno-economic analysis (TEA) provides more robust decision-making tools for PFAS treatment selection. The research addresses regulatory frameworks across jurisdictions, treatment media variability, and operational considerations. These insights enable water utilities, policymakers, and researchers to optimize PFAS remediation strategies by balancing economic constraints with environmental objectives, advancing more sustainable water treatment approaches.