Perfluoroalkyl substances (PFAS) exhibit excellent heat resistance, chemical resistance, insulating properties, and interfacial characteristics, rendering them indispensable in various industrial fields. However, the extremely strong carbon-fluorine (C-F) bond in these compounds leads to various environment-related challenges. For example, PFASs typically exhibit notable environmental persistence, and certain PFASs such as perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA) are highly bioaccumulative. Moreover, waste treatment of fluorinated compounds is challenging because the hydrogen fluoride generated by the combustion of fluorinated compounds deteriorates incinerators. Several techniques have been reported to decompose PFAS into recyclable fluoride ions, including oxidation using strong oxidants such as peroxydisulfuric acid and ultraviolet-C (UVC) irradiation (wavelength below 260 nm) using a mercury lamp under high temperature and pressure. Fluorine ions can be easily converted to calcium fluorides, which is a natural source of fluorine, and therefore, fluorine-recycling can be achieved. However, the use of mercury lamps as a light source is becoming less feasible owing to regulatory constraints imposed by the Minamata Convention on Mercury. A recent study demonstrates that perfluorooctanoic acid (PFOA) can be mineralized under strong basic conditions at 100 °C. However, such mild conditions are not suitable for the decomposition of more stable PFASs, such as PFOS and perfluoroalkyl polymers. Despite the widespread use of fluoropolymers in diverse industrial applications, their recycling rate remains low, and many of them are subjected to landfill burial. Therefore, it is necessary to develop a method to decompose extremely stable PFAS under mild conditions to address the multifaceted social issues linked with PFAS and to contribute to the realization of a sustainable fluorine-recycling society.