Polycarbonates (PCs) have been extensively blended with polyolefins such as polypropylene (PP) due to pecuniary advantages. Although the toughness of a pristine PC matrix has been examined, limited works have investigated the toughness of heterogeneous PC/PP blend systems, focusing merely on PC‐dispersed PP matrices. In this study, the mechanical/thermal properties of PP‐dispersed PC matrix (PC‐rich phase) were examined by using potential compatibilizers: poly(maleic anhydride‐alt‐α‐olefin) (OM), ethylene‐co‐acrylic acid (EA), and cyclic olefin copolymer. The incorporation of 0.5–5.0 phr of compatibilizers (OM and EA) into PC substantially enhanced the toughness of PC/PP15 blends according to four different testing methods. The highest toughness was obtained with 0.5 phr of OM and EA. The compatibilized blends displayed enhanced various thermal properties such as glass transition temperatures, heat deflection temperature, and degradation point, due to the compatibilizing effect. Moreover, 0.5 phr of compatibilizers (OM and EA) were determined as the most effective concentration in terms of toughness and most properties, without compromising strengths and moduli. The morphology of PP‐dispersed PC matrix (crystalline polymer‐infiltrated amorphous polymer matrix) differed from that of PC‐dispersed PP matrix. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47684.