We propose a new method of fabricating metal–polymer composite targets for sputtering, which makes it easier to control the composition and enables the homogeneous and reproducible fabrication of metal–polymer nanocomposites over large areas. Using Cu/polytetrafluoroethylene composite targets containing 20, 50, and 80 wt.% Cu, Cu/plasma polymer fluorocarbon (PPFC) nanocomposite thin films were prepared by radio-frequency (RF) sputtering. Targets with 80 wt.% Cu were conductive; moreover, sputtering was possible not only with RF but also with mid-range frequency (MF) and direct current (DC) power sources. The nanocomposite thin film deposited by MF and DC power using an 80 wt.% Cu target showed near-metallic characteristics, exhibited absorption peaks at 618 and 678 nm, and had a surface resistance of 2 × 104 and 34.55 Ω/sq, respectively. We also analyzed the structure and composition of the Cu/PPFC nanocomposite films by X-ray diffraction and X-ray photoelectron spectroscopy. The described metal–polymer targets can advance the applications and commercialization of nanocomposite thin films.