Poly- and perfluoroalkyl substances (PFAS) are surfactants. Leveraging their surface active feature, this work investigated using aeration to remove perfluoroalkyl acids (PFAAs) from aqueous solutions. Eight PFAAs were spiked to either deionized water or Hoagland solution at three pHs. After 7 h of aeration, removals of perfluorobutanoic acid (PFBA), perfluoropentanoic acid (PFPeA), perfluorobutanesulfonic acid (PFBS), and perfluorohexanoic acid (PFHxA) were marginal and much lower than those of and perfluoroheptanoic acid (PFHpA), perfluorohexanesulfonic acid (PFHxS), perfluorooctanoic acid (PFOA), perfluorooctanesulfonic acid (PFOS). In deionized water, close to 80% of PFOA and PFOS at 200 ppb were removed when the pH was 2.3. The Hoagland solution at pH 2.3 and 5.0 benefited removal of long-chain PFAS at 2 ppb, but not at 200 ppb. With duckweed growing on the Hoagland solution surface, >95% of PFHpA, PFHxS, PFOA, and PFOS at 200 ppb were removed after 2 weeks. Aeration enhanced duckweed uptake of PFHxS, PFOA, and PFOS at 2 ppb significantly. Specific to PFOS, duckweed accumulated 14.4% of this compound initially spiked at 2 ppb in 2 weeks. These results demonstrated that aeration plus duckweed could be a viable and scalable remediation solution for surface water contaminated by PFAS.