Per- and polyfluoroalkyl substances (PFAS) are a group of synthetic chemicals characterized with persistence and multisurface resistance. Their accumulation in the environment and toxicity to human beings have contributed to the rapid development of regulations worldwide since 2002. The sorption strategy, taking advantage of intermolecular interactions for PFAS capture, provides a promising and efficient solution to the treatment of PFAS contaminated sources. Hydrophobic and electrostatic interactions are the two commonly found in commercially available PFAS sorbents, with the fluorous interaction being the novel mechanism applied for sorbent selectivity. The main object of this Perspective is to provide a critical review on the current design criteria of PFAS sorbents, with particular focus on their sorption and interaction mechanisms as well as limitations. An outlook on future innovative design for efficient PFAS sorbents is also provided.