Blends of isotactic polypropene (i-PP) with random ethene/1-butene (EB) copolymers containing 10, 24, 48, 58, 62, 82, and 90 wt % 1-butene were prepared in order to examine the influence of the EB molecular architecture on the morphology development as well as on the thermal and mechanical properties. Compatibility between i-PP and EB increased with increasing 1-butene content in EB to afford single-phase blends at a 1-butene content exceeding 82 wt %. The morphology was investigated using AFM and TEM. Improved compatibility accounted for enhanced EB dispersion and interfacial adhesion. Highly flexible as well as stiff blends with improved toughness were obtained.