During nonisothermal crystallization of highly dispersed polypropylene/carbon nanotube (CNT) composites, considerable heterogeneous nucleation is observed to an extent scaling with the CNT surface area. Saturation occurs at higher loadings, reaching a plateau value for the crystallization onset which is 15 °C higher than in the unfilled matrix. Polymorphic behavior does not occur, as revealed from wide-angle X-ray diffraction. Upon subsequent heating, an increase in the melting temperature is observed due to increased crystalline perfection in the presence of CNTs. The complex multiple melting behavior is interpreted in terms of recrystallization phenomena. A study at varying heating and cooling rates reveals that CNTs affect the chain segment mobility of the matrix and largely inhibit recrystallization upon heating. TEM observation of the nanocomposite morphology evidences the occurrence of a transcrystalline layer around the CNTs. A structure model is presented, in which individually dispersed CNTs are separated from a bulklike polymer phase by a highly ordered crystalline interface with reduced polymer mobility.