The utilization of excess quantities as the basis of a thermodynamic approach can simplify the prediction of multicomponent data from binary ones. Whereas in Part II the excess formalism was applied to the prediction of liquid phase adsorption on solids, in this paper, the liquid/air interface is investigated. In order to show the generality of the suggested approach, thermodynamic equations are developed in analogy to Part II. Surface tensions are predicted by different excess models and compared with experimental data. From predicted surface tensions, ternary adsorption isotherms on the liquid/air interface are calculated. (C) 2004 Elsevier Inc. All rights reserved.