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Core–shell acrylic copolymer latexes containing bio resourced itaconic acid with different compositions in respect with the core and shell segments were synthesized, characterized, and applied as coating materials for leather. The purpose of the study was to evidence the high coating performance of the latexes when the ratio of the core/shell differed from 90/10 to 50/50 wt %. The copolymers were prepared via emulsion copolymerization technique and the products were isolated and characterized by means of structure identity, thermal behavior (DSC and DMTA), coating performance. The particle size of the latexes varied from 83 to 173 nm with the variation of the ratio of core/shell segments. The influence of the composition of soft part and hard part was highlighted in the thermal and coating properties. The optimal composition giving the best coating performance could be determined as DS 60/40. Further increase of the hard segment content, resulted in decreased emulsion stability and the coating performance on the leathers. The use of itaconic acid seemed to increase the emulsion stability as well the adhesion of the latexes to the substrate.