Two polypropylene cast films of different crystalline structures (one with coexisting small rows of lamellae and spherulites and the other with only a spherulitic structure) were prepared by extrusion. The produced cast films were uniaxially hot drawn at T = 120 degrees C using a machine direction orientation (MDO) unit and the changes in structure and morphology were examined and related to barrier as well as tear and puncture properties. Structural changes in terms of the degree of crystallinity and crystal size distribution, orientation of the amorphous and crystalline phases, and the deformation behavior at the crystal lattice and lamellae scales were investigated using differential scanning calorimetry (DSC), Fourier transform infrared spectroscopy (FTIR), wide angle X-ray diffraction (WAXD), and small angle X-ray scattering (SAXS), respectively. A significant effect of the original crystal morphology on the alignment of the amorphous and crystalline phases was observed from FTIR and WAXD. The results also revealed that the deformation behavior of the crystal structure was dependent on the draw ratio (DR). Our findings showed that by increasing DR the crystal lamellae first broke up and oriented along the drawing direction and then, at large DR, they were deformed and created a fibrillar structure. Morphological pictograms illustrating the effects of original morphology and draw ratio on the stretched film microstructure are proposed. The tear resistance along the machine direction (MD) decreased significantly with increasing DR whereas the puncture resistance increased drastically. Finally, the oxygen transmission rate (OTR) of the MDO stretched films could be correlated with the orientation parameters as well as the beta-relaxation peak magnitude of the amorphous tie chains. (C) 2009 Elsevier Ltd. All rights reserved.