This work is aimed at a predictive description of the thermodynamic properties of actinide(III) salt solutions at high concentration and 25 C. A new solution of the binding mean spherical approximation (BIMSA) theory, based on the Wertheim formalism, for taking into account 1: 1 and also 1: 2 complex formation, is used to reproduce, from a simple procedure, experimental osmotic coefficient variation with concentration for three binary salt solutions of the same lanthanide( III) cation: dysprosium( III) perchlorate, nitrate, and chloride. The relevance of the fitted parameters is discussed, and their values are compared with available literature values. UV-vis/near-IR, time-resolved laser-induced fluorescence spectroscopy experiments, and molecular dynamics ( MD) calculations were conducted for dilute to concentrated solutions (ca. 3 mol, kg(-1)) for a study of the microscopic behavior of DyCl3 binary solutions. Coupling MD calculations and extended X-ray absorption fine structure led to the determination of reliable distances. The MD results were used for a discussion of the parameters used in the BIMSA.