Ion-beam assisted deposition (IBAD) for Cr/Cu coatings was investigated. For high density and electric resistivity, IBAD was found to be an appropriate method. The density was increased from 8.60 g/cm3 to 8.85 g/cm3, depending on IBAD conditions, and the resistivity was increased from 6.4 μΩ·cm to 7.2 μΩ·cm. It is also suggested that the crystallographic orientations of polycrystalline Cu surfaces were able to be aligned to (111) planes by the IBAD process.