Growth and structural properties of thin a-C films prepared by the 60 MHz very-high-frequency (VHF) magnetron sputtering were investigated. The energy and flux of ions impinging the substrate were also analyzed. It is found that the thin a-C films prepared by the 60 MHz sputtering have a lower growth rate, a smooth surface, and more sp3 contents. These features are related to the higher ion energy and the lower ions flux onto the substrate. Therefore, the 60 MHz VHF sputtering is more suitable for the preparation of thin a-C film with more sp3 contents.