Per- and polyfluoroalkyl substances (PFAS), also known as “forever chemicals”, are manmade chemicals that have been increasingly detected in various geological media since the early 2000s. The soil and subsurface environments are the geological media commonly affected by PFAS. We conducted a comprehensive review of peer-reviewed studies published from 2010 through 2021 concerning the fate and transport of PFAS in subsurface environments. This review is organized into different subsections, covering the basics of PFAS properties and how they affect the occurrence, fate, and transport of PFAS, the fundamental processes affecting subsurface transport and fate of PFAS, and mathematical models for describing and predicting PFAS transport behaviors. Mechanisms governing PFAS transport in the subsurface environment, including the sorption of PFAS at the air‒water interface, solid‒water interface, and nonaqueous phase liquids‒water interface, were explored in detail. Challenges and future research priorities are identified to better combat the global challenges of PFAS contamination.