Per- and polyfluoroalkyl substances (PFAS) are a large group of engineered chemicals that have been widely used in industrial production. PFAS have drawn increasing attention due to their frequent occurrence in the aquatic environment and their toxicity to animals and humans. Developing effective and efficient detection and remediation methods for PFAS in aquatic systems is critical to mitigate ongoing exposure and promote water reuse. Adsorption-based removal is the most common method for PFAS remediation since it avoids hazardous byproducts; in situ sensing technology is a promising approach for PFAS monitoring due to its fast response, easy operation, and portability. This review summarizes current materials and devices that have been demonstrated for PFAS adsorption and sensing. Selectivity, the key factor underlying both sensor and sorbent performance, is discussed by exploring the interactions between PFAS and various probes. Examples of selective probes will be presented and classified by fluorinated groups, cationic groups, and cavitary groups, and their synergistic effects will also be analyzed. This review aims to provide guidance and implication for future material design toward more selective and effective PFAS sensors and sorbents.