In this study, high-density polyethylene films (HDPE) were produced using different processes (film blowing and biaxial orientation) and processing conditions. The orientation of the films was characterized in terms of their biaxial crystalline, amorphous and global orientation factors using birefringence, Fourier transform infrared spectroscopy (FTIR) using a tilted incidence technique and X-ray pole figures. Evaluation of a simplified FTIR procedure without using the tilted method for the determination of crystalline orientation factors proposed in the literature is also evaluated and assessed. The results indicate that FTIR overestimate the crystalline orientation factors, particularly for the crystalline a-axis. Significant discrepancies are also observed for the b-axis orientation, which may be due to an overlap of the amorphous contribution and/or saturation of FTIR bands. Those differences are larger for films with low orientation, such as blown films. Amorphous phase orientation from FTIR depends on the band used and is not necessarily in agreement with that determined from combination of X-ray and birefringence. Crown Copyright © 2005 Published by Elsevier Ltd. All rights reserved.