CrN/CNx nano-scale multilayered films were deposited on Si (100) substrate by closed-field unbalanced magnetron sputtering. Designed experimental parameters enabled an evaluation of the effects of negative substrate bias voltage (Vb), and bi-layer thickness λ (by changing substrate rotation rate) during deposition on the structural and mechanical properties of multilayer films. These multilayers were characterized and analyzed by transmission electron microscope (TEM), X-ray diffraction (XRD), atomic force microscopy (AFM), and nanoindentation measurements. In all cases, the CNx layers were amorphous and independent of Vb, while the microstructures of the CrN layers were dependent primarily on Vb. The CrN layers showed a mixed structure phase consisting of CrN, Cr2N, and Cr at Vb = -(40-120) V. At higher Vb values (-140 V or above), the Cr2N phase was dominant along with low CrN phase content. AFM measurements revealed that the root-mean-square (rms) surface roughness of the CrN/CNx film was 2 nm at Vb= -200 V whereas the rms values were about 9.5-3.3 nm for lower Vb values of -(40-180 V). By nanoindentation measurements, a maximum hardness of about 36 GPa was observed at Vb= -140 V. The improved mechanical properties of the films are correlated to the phase formation during deposition.