Modified and nonmodified blends of linear low-density polyethylene (PE) and polypropylene (PP) form separated phases of crystalline PP and PE. They form spherulitic crystals in the core, but highly oriented nonspherulitic phases at the skin of injection molded test bars. The dimension of the spherulites decreases with increasing PE content within the blends. Crystallization behavior of both crystalline phases is influenced by the other phase. The crystallization temperature of PP is increased in the presence of the compatibilizer. Transmission electron micrographs of blends modified by poly(styrene-block-ethylene/butylene) (SEBS) and stained by OsO4 showed co-continuous lamellar structure of the blends with a polypropylene phase containing the majority of the modifier. Smaller portions of the modifier can be found on the surface of the two olefinic phases as dispersed spheres, with an average diameter of 50-90 nm. The lamellar structure is independent of the spherulitic structure, and interpenetrates the spherulites. The conclusion of this study is that this block copolymer, while improving the physical properties of the blends, is not a true compatibilizer of the system according to the conventional terminology of physical chemistry.