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The effects of morphology on the barrier properties of poly(ethylene terephthalate) (PET) have been investigated. Various levels of crystallinity can be developed in PET as a result of thermal exposure, orientation, and heat setting. The morphologies of the crystalline phase are affected by the conditions of their formation. As a result of morphological differences, samples with equivalent levels of crystallinity have been found to exhibit different oxygen barrier properties. These differences are most apparent at low and intermediate levels of crystallinity. For thermally crystallized systems, at the same crystalline content, increasing superstructure size in the crystalline phase leads to greater tortuosity for the permeant molecules, resulting in lower permeability. For stretched and heat set PET, transport properties can be correlated with birefringence as well as overall orientation, measured in terms of fraction of molecules in the trans or extended chain conformation. At high levels of crystallinity, where the spherulites become volume filling, permeation takes place primarily through the interlamellar regions of the crystalline phase and is controlled by level of crystallinity, independent of the mode of crystallization. The barrier properties of PET, before spherulitic impingement occurs, are governed by the size and number of spherulites as well as by the amorphous orientation present in non‐crystalline regions. POLYM. ENG. SCI., 45:400–409, 2005. © 2005 Society of Plastics Engineers