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Polytetrafluoroethylene (PTFE) has many excellent engineering applications for its great properties. We investigated the surface of the PTFE membranes treated with atmospheric pressure low temperature plasma in Ar and Ar/H2 to confirm the effectiveness for introducing functional groups as surface modifications. From the results of attenuated total reflection (ATR) Fourier transform infrared (FT-IR) spectroscopic analysis and X-ray photoelectron spectroscopy (XPS), it was found that the Ar/H2 plasma was more effective for proceeding defluorination reactions and introducing oxygen moieties compared to Ar plasma under the experimental condition. On the other hand, from the results of scanning electron microscopy (SEM), there were little differences in plasma-treated samples.