A new synthesizing method, IR-laser-assisted electron-cyclotron-resonance plasma-enhanced chemical vapor deposition (LA-ECR-PECVD), has been used to fabricate Si-C-N and C-N films on steel substrates at low temperatures (< 650 °C). Methane/nitrogen or carbon dioxide/nitrogen gases are dissociated to methane radicals and nitrogen plasma by the IR-laser and ECR to enhance the species' energy. An IR-laser beam (pulsed Nd:YAG laser, 1064 nm) was introduced into the growth chamber for two purposes: (1) to add Si atoms by ablating a Si target, and (2) to enhance the plasma concentration in the gas phase. An infrared vibration mode located at 1256 cm-l wavenumber was observed in Si-C-N and C-N films, although these films have an amorphous phase. The C-N film also has a Raman shift at 1276 cm-l. The AFM images reveal many islands with a size ranging from 50 nm – 150 nm in films.