The deposition of nitrogen-containing carbon films on silicon substrates at atmospheric pressure and low temperature has been carried out by electrolysis of methanol and ammonia solutions. Amorphous carbon films containing about 8% nitrogen were obtained. The observed CN vibration bonds by Raman and FTIR spectroscopy and the chemical states by XPS of C and N atoms indicate that the carbon and nitrogen are sp(2) and sp(3) chemically bonded in the films. Schemes for film growth in the liquid phase were suggested.