PFAS adsorption by nanoparticles (NPs) is an important determinant of their fate in the environment. A deeper insight into their interaction, especially under complex conditions, is still lacking. Here, we first found that the inherent properties of PFASs (e.g., concentration and chain length) strongly determine their interaction with carbon NPs (CNPs) in aquatic environments under different ionic strengths. With an identical increase in the ionic strength, more enhancement (255%) in the association ability of CNPs was achieved with long-chain PFAS at a high initial concentration (10 mg/L) compared with that at a lower initial concentration (6%, 0.1 mg/L), while the situation of short-chain PFASs was the opposite (36 vs 557%). The effect of ionic strength on hydrophobic interactions was proved to be the origin of the above phenomenon. A high ionic strength induces the formation of hydrogen bond networks of water molecules, which enhances hydrophobic interactions. However, when the PFAS concentration is lower, hydrogen bond networks are more difficult to organize around PFAS molecules, weakening the positive effect of the ionic strength. Moreover, the solvation of long-chain PFASs in water is thermodynamically unfavorable at high ionic strength, making them "easily excluded". This is a brand new insight into the interaction between PFASs and NPs under complex aquatic conditions, which will be meaningful to predict the fate of PFASs in the environment.