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Organic semiconductors (OSCs) are of interest for replacing traditional Si-based semiconductors as their flexibility and transparency enable new applications. The properties of OSC materials greatly depend on their orientation and molecular arrangement, which are strongly dependent on the underlying substrate material. Hence, in this study, in situ ultraviolet photoelectron spectroscopy (UPS) is used to elucidate the effect of the substrate on OSC orientation. Two types of OSCs, namely those with shape anisotropy (pentacene, dinaphtho[2,