On the basis of daily Saharan dust samples collected at Sal Island (Cape Verde Archipelagos) and Barbados (Caribbean Sea) over 3 years, this study focuses on the mineralogical signature of the African sources providing dust over the tropical North Atlantic Ocean. First, the sources of the collected dust were localized by using relative clays abundance (illite-to-kaolinite ratio) combined with Meteosat infrared imagery, horizontal visibility, and backward trajectories of dusty air masses. Then, each identified source was linked to a single value of the illite-to-kaolinite ratio. Those results highlight that the clay content of the emitted dust depends directly on both the latitude and the longitude of the source. Dust originating from northwestern sources exhibits illite-to-kaolinite ratios higher than those from Sahelian regions. Likewise, illite-to-kolinite ratio decreases from west to east.