Perfluoroalkyl and polyfluoroalkyl substances (PFASs) pollution with their toxicity, carcinogenicity, and persistence has been concerned worldwide. Research into novel materials for detecting and removing PFASs has increased rapidly, particularly in regard to the emergence of well-characterized single-atom materials (SAMs). Owing to the high selectivity, high atom utilization, and abundant active sites of SAMs, these materials exhibit remarkable efficacy in the detection and removal of PFASs. In this work, recent advances in the synthesis of SAMs for the detection and removal PFASs are reviewed. In-depth discussions of the structure-activity relationship and reaction mechanisms have demonstrated the high efficiency, activity, and selectivity of SAMs for the detection, adsorption, and degradation of PFASs. To optimize the application of SAMs in PFASs remediation, this review comprehensively surveys SAMs applications for PFASs and analyzes potential design strategies based on synthesis methods and corresponding properties. Synthesis strategies such as wet-chemistry, which offer ease of operation and high potential for large-scale production, are recommended for the further exploration of specific SAMs for the detection and removal of PFASs. Finally, this review identifies the challenges and opportunities for development of SAMs for the detection and remediation of PFASs, providing an outlook on strategic goals for a green economy and sustainable development. (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(PFASs)(sic)(sic)(sic)(sic)(sic)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)PFASs(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)(sic)(SAMs)(sic)(sic)(sic)(sic)(sic)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic), (sic)PFASs(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)PFASs(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)PFASs(sic)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic);(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)PFASs(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)PFASs(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).