Water pollution has emerged as one of the most urgent environmental concerns worldside. Per-and polyfluoroalkyl substances (PFASs) are widely used in the production of semiconductors, electronic products, and foam fire extinguishers. However, their high toxicity, persistence, bioaccumulation, and long-range transportability pose severe threats to both human health and the environment. Consequently, the development of detection and removal techniques for PFASs has become a paramount focus in today's society. Fluorescence detection stands out as a promising method due to its high sensitivity, simplicity, visual clarity, and affordability compared to traditional detection methods. Furthermore, traditional adsorbents such as activated carbon and ion exchange resins often exhibit low selectivity, poor adsorption capacity, and slow adsorption rates for PFASs. Therefore, there is an urgent need to develop new materials that can achieve rapid and sensitive detection as well as efficient removal of PFASs. Supramolecular macrocycles, as an emerging class of multifunctional materials, possess numerous advantages such as rich host-guest molecular recognition, good environmental adaptability, and designable structures. The designability of supramolecular macrocycles endows them with specific multifunctionality. These features make them an ideal platform for simultaneous detection and removal of PFASs from water environments. This review summarizes the applications of supramolecular macrocycles and their derivatives in the detection and adsorption of PFASs. It starts by introducing common classifications of PFASs and then delves into specific supramolecular structures that demonstrate high adsorption efficiency for PFASs, along with their corresponding adsorption mechanisms. Additionally, the review presents methods for regenerating supramolecular adsorbents, and offers insights into the design strategies for next-generation supramolecular materials with improved PFASs removal performance.