A short review about the structure, condition of formation, and reorganization behavior of the mesophase of isotactic polypropylene, summarizing recent work of the authors, is provided. Emphasis is put on the presentation of data collected by novel analysis techniques like fast scanning chip calorimetry (FSC), temperature-resolved X-ray analysis, or temperature-resolved atomic force microscopy (AFM), for quantitative characterization of the kinetics of the liquid-mesophase transition and of the conversion of the mesophase into crystals. In addition, the impact of crystallization of polypropylene via intermediate formation of a mesophase on engineering properties will be highlighted.