In the present study, the Raman spectra of diamond-like amorphous (a-C) and hydrogenated amorphous (a-C:H) carbon films on silicon obtained using the ion-beam methods and the pulse cathodic arc deposition technique were investigated with the aim of elucidating the relation between the hardness and structure of the films. The hardness of the samples used in the present study was 19-45 GPa. Hydrogenated carbon films were synthesized using END-Hall ion sources and a linear anode layer ion source (LIS) on single-crystal silicon substrates. The gas precursors were CH4 and C3H8, and the rate of the gas flow fed into the ion source was 4.4 to 10 sccm. The ion energies ranged from 150 to 600 eV. a-C films were deposited onto Si substrates using the pulse cathodic arc deposition technique. The films obtained by the pulse arc technique contained elements with an ordered structure. In the films synthesized using low-(150 eV) and high-energy (600 eV) ions beams, an amorphous phase was the major phase. The significant blurriness of the diffraction rings in the electron diffraction patterns due to a large film thickness (180-250 nm) did not allow distinctly observing the signals from the elements with an ordered structure against the background of an amorphous phase.