Oceanic bromoform (CHBr3) is the major source of organic Br to the atmosphere and may be significant for ozone depletion through the contribution of reactive bromine to the upper troposphere and lower stratosphere of the midlatitudes and tropics. We report the first analyses of boundary layer air, surface and deep ocean waters from the tropical Atlantic. The data provide evidence of a source of CHBr3 throughout the tropical open ocean associated with the deep chlorophyll maximum within the tropical thermocline. Equatorial upwelling carries the CHBr3 to the surface, adding to increased concentrations in the equatorial mixed layer and driving oceanic emissions that support locally elevated atmospheric concentrations. In air masses that had crossed the coastal upwelling region off NW Africa even higher atmospheric mixing ratios were measured. The observations suggest a link between climate, wind‐driven upwelling, and the supply of Br to the upper atmosphere of the tropics.