With the recent development of foldable electronic devices, there is a growing demand for display materials that exhibit resistance to the formation of fold marks (folding resistance). While polyethylene terephthalate (PET) films biaxially stretched in machine direction (MD) and transverse direction (TD) are commonly used as display films, they have poor folding resistance, especially when folded in the strongly stretched direction. Therefore, we aim to elucidate the primary factors behind fold mark formation in PET films, focusing on the anisotropy of the folding resistance. To analyze the aggregation structure changes resulting from bending deformation, synchrotron X-ray scattering measurements (ultrasmall, small, and wide-angle X-ray scattering; USAXS, SAXS, and WAXS) were performed. The PET films strongly stretched in the TD direction were kept folded in either MD or TD direction, and X-rays were irradiated in the surface normal or edge direction of the film to analyze their structure changes from various angles. As a result, in the convex region, the normal direction of the lamella coincided with the direction of the principal stress, whereas in the concave region, it was inclined at a 40−45°angle to the principal stress. On the other hand, the (100) plane of the crystal lattice maintained its orientation parallel to the film surface from convex to concave, although the orientation was slightly disrupted in the concave region. These results suggest that polymer chains slip parallel to the chain direction, causing no change in the orientation of the polymer chains but only the normal of the lamellar surface. When the PET films were folded in the TD direction, which shows poor folding resistance, the formation of a tilted lamellar surface was more pronounced compared to MD folding. Given that the formation of transformed lamellae caused by the chain slip is related to plastic deformation, which leads to permanent strain, this deformation contributes to the formation of fold marks. As the molecular chains are oriented in the strongly stretched direction, TD direction, it is assumed that they are more susceptible to forming kinks and yielding when subjected to compressive deformation within the concave region.