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Abstract Carbon nanotube/polytetrafluoroethylene composite polymer targets are proposed for use in the fabrication of fluorocarbon thin films using the mid-frequency sputtering process. Fluorocarbon thin films deposited using carbon nanotube/polytetrafluoroethylene composite targets exhibit an amorphous phase with a smooth surface and show a high water contact angle, optical transmittance, and surface hardness. X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy studies reveal that as the carbon nanotube concentration increased in the composite target, a carbon cross-linked structure was formed, which enhanced the film hardness and the modulus of the fluorocarbon thin film. Large-area fluorocarbon thin films with a substrate width of 700 mm were successfully fabricated by a pilot-scale roll-to-roll sputtering system using a carbon nanotube/polytetrafluoroethylene composite target.