The article represents the results of research in self-organization of new lanthanide systems in water-decanol medium. The systems are based on N,N-dimethyldodecylamine oxide, a zwitterionic surfactant. The study covers the complex formation of lanthanide ions with C12DMAO molecules and the influence of Ln(III) ions and medium composition on surfactant association in diluted solutions. The analysis of adsorption isotherms was carried out on the basis of the combination of Gibbs and Langmuir adsorption equations. The results were used to determine physicochemical properties and parameters of a monomolecular adsorption layer. The research objects were various lanthanide ions with identical coordination centers. A number of spectroscopic methods (UV, NMR self-diffusion, EPR, dynamic light scattering (DLS), and fluorescent analysis) were involved in the research for comparative estimations of molecular dynamics, critical micellization concentration, geometry, sizes, and aggregation numbers of micellar aggregates. Micelle structure simulation revealed good agreement between experimental data and quantum chemical calculations.