This study mainly focuses on the formation of isotactic polypropylene (iPP) blend morphologies with microspheres and distinct bead-string spherulites. iPP microspheres have been prepared by a simple and convenient strategy through either an isothermal or a nonisothermal crystallization process based on the macrophase-separated structure in molten state of iPP/olefin block copolymer (OBC) blend. The dimension of the iPP spheres can be adjusted easily from about 1 mm to >10 mm by controlling the compatibility and annealing conditions. It was found that any of the following three parameters, the molecular structure of OBC (particularly the octene content), molecular weight of iPP, and annealing condition can be rescaled with others in controlling the dimension of the iPP microspheres. The mechanism of the formation of iPP microspheres was studied in detail. Surprisingly, the typical spinodal decomposition morphology with interconnected or thin sheet structure is the precursor of these microspheres. During the subsequent annealing process, it breaks up and further coarsens into spherical structure. In addition, distinct spherulites with a bead-string substructure have been obtained during the isothermal crystallization.