A series of VC/TiN nano-multilayer films with various TiN layer thicknesses were synthesized by magnetron sputtering method. The relationship between the modulation structure and superhardness effect of the multilayer films were investigated. The results reveal that TiN below a critical layer thickness grows coherently with VC layers in multilayers. Correspondingly, the hardness and elastic modulus of the multilayers increase significantly. The maximum hardness and modulus achieved in these multilayers is 40.7GPa and 328GPa.With further increase in the TiN layer thickness, coherent structure of multilayers are destroyed, resulting in a remarkable decrease of hardness and modulus. The superhardness effect of multilayers is related to the three directional strains generated from the coherent structure.