Wet deposition and dry deposition of legacy per- and polyfluoroalkyl substances (PFAS) and perfluoroalkyl ether carboxylic acids (PFECAs) were assessed on the southeastern coast of the United States, specifically, in Wilmington, NC, which is located 110 km from a fluorochemical manufacturer. Analytes were quantified by liquid chromatography coupled to electrospray ionization with triple-quadrupole mass spectrometry. Total concentrations of six PFAS compounds ranged from below the method quantification limit to 110 ng L–1 by wet deposition, and total fluxes of 0.3–29 ng m–2 day–1 by dry deposition were found. The estimated annual flux of all six PFAS was 30 μg m–2 by wet deposition and 1.4 μg m–2 by dry deposition, indicating that PFAS are more effectively removed from the atmosphere by wet deposition. There was a significant rainout/washout effect observed in our data, but there was no impact of the origin of the air mass on concentration or flux, suggesting that the incorporation of PFAS into rainwater is a relatively local phenomenon. This study shows the first direct evidence of PFECAs in wet and dry deposition. The data suggest that the particle-bound and gas-phase PFAS that may have undergone long-range transport can be incorporated into raindrops and removed rapidly.