Dry deposition is an important yet poorly constrained process that removes reactive organic carbon from the atmosphere, making it unavailable for airborne chemical reactions and transferring it to other environmental systems. Using an aircraft-based measurement method, we provide large-scale estimates of total gas-phase organic carbon deposition rates and fluxes. Observed deposition rates downwind of large-scale unconventional oil operations reached up to 100 tC hour-1, with fluxes exceeding 0.1 gC m-2 hour-1. The observed deposition lifetimes (τdep) were short enough (i.e., 4 ± 2 hours) to compete with chemical oxidation processes and affect the fate of atmospheric reactive carbon. Yet, much of this deposited organic carbon cannot be accounted for using traditional gas-phase deposition algorithms used in regional air quality models, signifying underrepresented, but influential, chemical-physical surface properties and processes. Furthermore, these fluxes represent a major unaccounted contribution of reactive carbon to downwind freshwater ecosystems that outweigh terrestrial sources, necessitating the inclusion of dry deposition in aquatic carbon balances and models.