Polyethylene terephthalate (PET) is one of the most used polymeric substances in production of packaging materials, fibers, textiles, coatings, and engineering materials. This paper elucidates the transport parameters of hydrogen gas through a PET membrane, which was selected to be a sufficiently permeable substrate for setting up an empirical strategy that aims at developing hydrogen barrier coatings. An examination of the structural degradation of PET by prolonged hydrogen exposure was performed. Hydrogen permeation tests were performed on a PET membrane with a thickness of 50 μm. To investigate the behavior of the material by prolonged hydrogen treatment, hydrogen-exposure experiments were carried out at a certain hydrogen pressure and time. Comparisons of the mechanical properties of the material were documented both before and after hydrogen exposure. A strong impact of comparatively transient hydrogen exposure on the mechanical and hydrogen transport properties of PET was observed. After 72 h of hydrogen exposure at 103 hPa and 300 K, the tensile strength decreased by 19%, the diffusion coefficients more than doubled, and material fracture behavior changed from ductile to distinctly brittle. This underlines the importance of developing effective hydrogen barrier coatings in case PET tubing is intended for use in hydrogen transport or storage.