Calcium carbonate (CaCO3) fillers pre-treated with the increased amount of stearate were used in order to tune the surface energy for a selective filler migration to the interface in immiscible styrene-acrylonitrile/ethylene–propylene–diene (SAN/EPDM) polymer blends. Various models were used in order to predict the filler accommodation at the blend interface when the interfacial tension becomes low and the wettability is good. The results showed that under optimal thermodynamic conditions, the filler might act as a compatibilizer and significantly improve the blend morphology. The coarse morphology of the initially immiscible SAN/EPDM changed into a fine blend morphology with the addition of the selected CaCO3 fillers with optimal surface energy. Due to the problem with filler agglomeration of initially nanosized CaCO3 fillers, we used masterbatch (MB) compositions for the blend preparation in order to get the better filler distribution. In this paper, the comparison between two types of MB compositions based on SAN and/or EPDM as a surplus phase with the selected filler was made considering the model predictions and its effects on the blend morphology and properties. In the case of using MB(EPDM) in blend preparation, the fine blend morphology resulted in improved mechanical and thermal properties, while with MB(SAN) the coarse blend morphology and worsened properties illustrated the opposite effect.