A hybrid process of pulsed plasma-based ion implantation and deposition using two kinds of hydrocarbon plasma C 2 H 2 and C 6 H 5 CH 3 was developed to produce diamond-like carbon (DLC) films, respectively. A residual stress of each film was measured as a function of negative pulsed voltage. The residual stress of the DLC film prepared by the C 6 H 5 CH 3 plasma with −5 kV negative pulsed voltage reduced to 0.005 GPa. The microstructure of the DLC films prepared by the C 2 H 2 and the C 6 H 5 CH 3 plasma was investigated. In the case of C 2 H 2 plasma deposition with −20 kV negative pulsed voltage, only an amorphous film was formed. In the process of deposition by C 6 H 5 CH 3 with −10 kV negative pulsed voltage, some fine particles were found in the amorphous film, which had a geometric shape, and the diameters of these particles were from 30 nm to 50 nm. It was found that they had the crystal structure of carbon (168H), which has the lattice constant of 0.32, 0.25, 0.2 and 1.9 nm. The formation of these carbon particles in the DLC film might be due to the generation of glow discharge.