Carbon nitride (CN) films were synthesized on silicon substrates by a combined ion-beam and laser-ablation method under various conditions; ion-beam energy and ion-beam current were varied. Raman spectroscopy and spectroscopic ellipsometry (SE) were employed to characterize respectively the structural and the optical properties of the CN films. Raman spectra show that all the CN films are amorphous independent of the ion-beam current and the ion-beam energy. Refractive indices, extinction coefficients and optical band gaps which were determined from the measured SE spectra exhibit a significant dependence on the synthesis conditions. Especially, the decrease of the refractive indices and the shrinkage of the optical band gap is noticeable as the ion-beam current and/or the ion-beam energy increase.