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A surface modification technique that improves the adhesion of fluorocarbon polymer films such as polytetrafluoroethylene (PTFE), perfluoroalkoxy fluoroplastics, and polychlorotrifluoroethylene is developed using argon at atmospheric pressure and acrylic acid vapor nonthermal plasma. The results of the T-type peeling test show that the peeling strength of the treated PTFE film is approximately 70 times greater than that of the untreated film. From X-ray photoelectron spectroscopy and scanning electron microscope analyses, it is confirmed that chemical bonds with F atoms decrease greatly on the surface and that a hydrophilic layer is formed due to the plasma graft polymerization process. Using the present surface treatment apparatus, it is possible to bond A4-sized sheets of PTFE and metals without losing the excellent physical properties of PTFE.