Atmospheric particulate matter samples were collected from mid-Atlantic and northeastern U.S. (Virginia and New York, respectively) sites to assess the fossil versus contemporary sources contributing to aerosol organic carbon (OC) and the implications for its deposition to watersheds. Mean particulate matter total OC (TOC) deposition rates (wet + dry deposition) were calculated to be 1.6 and 2.4 mg C m−2 d−1 for the Virginia and New York sites, respectively. Wet deposition of particulate TOC was determined to be the dominant depositional mode, accounting for >65% (Virginia) and >80% (New York) of total aerosol TOC deposition. Isotopic mass balances suggest that, on average, the deposited aerosol TOC consisted of 66% (Virginia) and 68% (New York) contemporary biomass-derived material. The balance was fossil-derived material (34% and 32% for Virginia and New York, respectively), indicating significant anthropogenic fossil fuel contributions to aerosol TOC. When considered within representative northeastern U.S. watershed OC budgets, aerosol TOC depositional flux was up to 10% of net soil OC accumulation rates, and 5–70% of the OC throughfall flux for forested regions. When scaled to the entire Hudson and York River watersheds, estimated aerosol TOC depositional fluxes ranged from 6.1 to 9.7 × 1010 g C yr−1 and from 8.9 to 14 × 109 g C yr−1, respectively, and were similar in magnitude to the mean annual river OC export for these two systems (Hudson, 7.2 × 1010 g C yr−1; York, 8.4 × 109 g C yr−1). These findings underscore the potential importance of both natural and fossil fuel-derived aerosol OC inputs to watersheds.