Abstract: Multi-layer composite films consisted of C₆₀ and diamond-like carbon (DLC) can be prepared on Si, glass and other substrates by vacuum sublimation deposition followed by radio-frequency chemical vapor deposition (RFCVD) method with the CH₄ and H₂ gas as the reactants. The films and their characteristics were identified by Raman spectra. The resistivity and dielectric constant of the films were studied by means of a LF impedance analyzer so as to obtain the relationship between the frequency and the dielectric constant and resistivity of the films. The results show that resistivity of the films under the various frequency are approximately consistent with a pure C₆₀ film, but the permittivity varied with the frequency for the pure C₆₀ film is obviously distinguished from the composite films. The phenomena and results were discussed and analyzed by Debye's model and dielectric relaxation theory. And then according to the corresponding simulating formula, the relationship between the experimental dielectric constant and frequency was fitted by the computer calculation to gain the relaxation time, dielectric constant etc. The fitted results are basically consistent with the experimental data.