Per- and polyfluoroalkyl substances (PFAS) are a class of toxic and bioaccumulative compounds affecting environmental and human health. Conventional wastewater treatment processes are ineffective at remediating these persistent chemicals. While functional framework materials have been shown to remove PFAS via adsorption and catalytic degradation, there is an on-going debate about their practical use in water purification. Inspired by recent research on typical functional framework materials, including zeolites, metal-organic frameworks (MOFs), and covalent organic frameworks (COFs), our review summarizes the principles of their design, properties, and applications with a special emphasis on PFAS removal. The potential of framework material for catalytic degradation of PFAS is constructively discussed, based on limited studies thus far. Finally, the challenges of using framework materials to remove and degrade PFAS in wastewater are presented along with sustainable design prospects to improve the technology. The current review provides new insights in advancing framework materials for PFAS elimination from contaminated waters.