The casein micelle is a highly aggregated colloid consisting of phosphoproteins and minerals, in particular calcium and phosphate. Its properties are affected by physico-chemical changes which provide possibilities for the development of new casein aggregates (CAs) with novel functionalities. The aim of this study was to investigate the emulsifying and emulsion-stabilizing capacity of gradually demineralized CAs in model dairy emulsions. Tri sodium citrate (TSC) was used to remove calcium and inorganic phosphate from pure casein micelles in order to produce four suspensions of differently demineralized CAs. Two types of milkfat-in-suspension (30:70 v/v) emulsions were then prepared to study the emulsifying and emulsion-stabilizing capacity of these CAs separately. Casein micelles were progressively demineralized (from 24 to 81% calcium reduction) and dissociated with the increase in TSC concentration. Three distinct populations of particles (micelle-like aggregates, sodium caseinate-like aggregates and casein monomers) were present in every suspension in different proportions. The smaller CAs had better emulsifying capacity and similar surface activity according to interfacial studies. The state of aggregation of the CAs was thus the main factor that controlled their emulsifying capacity. However, the emulsions formed with these smaller aggregates were less stable against creaming and flocculation, but still resisted coalescence under our storage conditions (21 days at 50 °C). The properties of the interfacial casein layers did not depend on the aggregation state of the CAs used to form the emulsions. The differences in instability were attributed to the nature of the non-adsorbed CAs and storage conditions.