Per- and polyfluoroalkyl substances (PFASs) include thousands of fluorinated organic compounds of anthropogenic origin. Their extensive use, combined with their high stability, has led to the widespread contamination of water and soil resources. Here, single-step foam fractionation enhanced soil washing was carried out for the remediation of PFAS-contaminated soil. Concentrations of target Perfluoroalkyl Carboxylic Acids (PFCAs) and Perfluoroalkane Sulfonic Acids (PFSAs) were monitored in foam and leachate along the duration of the treatment. Among PFCAs, only long-chain compounds peaked in foam at the beginning of the treatment. This was consistent with the increase in the sorption affinity to the air–water interface with chain length. The same behavior was observed also in PFSAs by comparing PFHXs, PFHpS and PFOS. The fraction of PFCAs still in the leachate after 40 min of treatment was found to decrease with chain length, with PFSAs showing a similar trend. PFAS removal significantly increased with soil particle size, ranging from 48.2 ± 3.2% (fraction < 0.063 µm) to 64.1 ± 1.9% (fraction > 2 mm). Final mass balance analyses detail PFAS distribution among soil, leachate, and foam, providing valuable information for the additional treatment required to destroy the PFAS load extracted from the contaminated soil.