The compositions of the adsorbed aggregates at the mica-solution interface have been directly determined for mixtures of pyridinium. chloride hydrocarbon and fluorocarbon surfactants by solution depletion measurements, including direct determination of the adsorbed layer composition for partially miscible surfactants. The measured adsorbed aggregate compositions are compared with predictions for bulk micelles using the group contribution method and regular solution theory. For fully miscible surfactants, there is good agreement between the models and experimental results. The group contribution method successfully predicts the existence of a miscibility gap for some mixtures, but adsorption experiments reveal some unusual features; the adsorbed layer consists of only one of the two coexisting micelle compositions, and its composition differs from that predicted. This effect is attributed to the substrate.