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Combined photoemission and charge-transport property studies of the organic hole transport material 2,2',7,7'-tetrakis(N,N-di-p-methoxyphenylamine)-9,9'-spirobifluorene (spiro-MeOTAD) under air exposure and controlled environments of O2, H2O + N2, and N2 (1 atm and under dark conditions) reveal the incorporation of gas molecules causing a decrease in charge mobility. Ultraviolet photoelectron spectroscopy shows the Fermi level shifts toward the highest occupied molecular orbital of spiro-MeOTAD when exposed to air, O2, and H2O resembling p-type doping. However, no traces of oxidized spiro-MeOTAD(+) are observed by X-ray photoelectron spectroscopy (XPS) and UV-visible spectroscopy. The charge-transport properties were investigated by fabricating organic field-effect transistors with the 10 nm active layer at the semiconductor-insulator interface exposed to different gases. The hole mobility decreases substantially upon exposure to air, O2, and H2O. In the case of N2, XPS reveals the incorporation of N2 molecules into the film, but the decrease in the hole mobility is much smaller.