Nanocomposites of isotactic polypropylene (iPP) and multiwalled carbon nanotubes (MWCNTs) with various contents of MWCNTs were fabricated by double molding techniques. X-ray diffraction measurements reveal a development of a-crystal with lamellar stacks having a long period of 150 Å in the neat iPP that increases to 165 Å in 2 wt % MWCNTs-loaded composites, indicating that MWCNTs enhance crystallization of iPP as a nucleating factor. Mechanical properties, such as tensile strength, flexural strength, Young's modulus, tangent modulus, and microhardness are found to increase with increasing MWCNTs content. Thermal analyses represent an increase of crystallization and melting temperatures and a decrease of thermal stability of the composites with increasing MWCNTs. Changes in structural, mechanical, and thermal properties of the composites due to the addition of MWCNTs are elaborately discussed.