Hydrogenated carbon films were synthesized on single-crystal silicon substrates by an END-Hall ion source or by a linear anode layer source. The gaseous precursors were CH4 and C3H8. The flow rates ranged from 4.5 to 10 sccm. In films synthesized from ion beams, amorphous phase was most pronounced. Carbon films were deposited onto silicon using pulse cathodic arc technique. In these films ordered-structure elements were identified. Raman spectra of a-C and a-C:H films were investigated with the aim of elucidating the interrelation between the hardness of the films (which reached 18, 20, and 45 GPa) and their microstructure.