We report aerosol ammonium 15N signatures for samples collected from research cruises on the South Atlantic and Caribbean using a new high sensitivity method. We confirm a pattern of isotopic signals from generally light (δ15N −5 to −10‰), for aerosols with very low (<2 nmol m−3) ammonium concentrations from the remote high latitude ocean, to generally heavier values (δ15N +5 to +10‰), for aerosols collected in temperate and tropical latitudes and with higher ammonium concentrations (>2 nmol m−3). We discuss whether this reflects a mixing of aerosols from two end-members (polluted continental and remote marine emissions), or isotopic fractionation during aerosol transport.