Qualitatively and quantitatively, we have demonstrated that airborne polychlorinated biphenyl (PCB) concentrations in the air surrounding New Bedford Harbor (NBH) are caused by its water PCB emissions. We measured airborne PCBs at 18 homes and businesses near NBH in 2015, with values ranging from 0.4 to 38 ng m-3, with a very strong Aroclor 1242/1016 signal that is most pronounced closest to the harbor and reproducible over three sampling rounds. Using U.S. Environmental Protection Agency (U.S. EPA) water PCB data from 2015 and local meteorology, we predicted gas-phase fluxes of PCBs from 160 to 1200 μg m-2 day-1. Fluxes were used as emissions for AERMOD, a widely applied U.S. EPA atmospheric dispersion model, to predict airborne PCB concentrations. The AERMOD predictions were within a factor of 2 of the field measurements. PCB emission from NBH (110 kg year-1, average 2015) is the largest reported source of airborne PCBs from natural waters in North America, and the source of high ambient air PCB concentrations in locations close to NBH. It is likely that NBH has been an important source of airborne PCBs since it was contaminated with Aroclors more than 60 years ago.