Wet atmospheric deposition and throughfall samples were collected weekly and analyzed for 33 per- and polyfluoralkyl substances (PFAS) during April through November 2023 within an old growth forest in the New York Botanical Garden. The median total PFAS concentration in throughfall during the study period was 7.43 ng/L, 5.7 times greater than the median total PFAS concentration in wet deposition. The median total atmospheric deposition of PFAS in throughfall was 21.74 ng/m²/d, 3.4 times greater than wet deposition highlighting the dominance of dry deposition of PFAS over wet deposition to this urban forest. Perfluorobutanoic acid (PFBA) had the highest concentration among the PFASs, and carboxylates (PFCAs) were the dominant group in both forms of atmospheric deposition. Short chain PFASs were dominant in wet deposition and throughfall, though to a lesser extent in throughfall. Precipitation amount was significantly and inversely correlated with several of the PFASs in wet deposition, and this relationship was stronger in throughfall consistent with atmospheric scavenging and particle wash-off as processes affecting atmospheric PFAS deposition. Several major ions in wet deposition and throughfall, most notably Ca²⁺, were significantly and positively correlated with several of the PFASs, providing additional evidence that atmospheric scavenging and particle wash-off are important processes affecting atmospheric deposition to the study forest. These results indicate that dry deposition of PFAS as reflected in throughfall is the dominant form of atmospheric deposition to this urban forest. Further studies are warranted to examine the role of throughfall in other forested settings.