This article presents the application of the response surface methodology for yielding the optimal conditions and for developing robust surface morphologies of zirconium nitride (ZrN) films. In this research, the ZrN films with (Ti, Cr) interfaces ((Ti, Cr)ZrN) were prepared by an unbalanced magnetron (UBM) sputtering. Two kinds of zirconium nitride films, with and without Ti additives, were reported. An orthogonal array for reducing the large number of experiments was introduced. The significant parameters from an analysis of variance for the (Ti, Cr)ZrN films were clearly observed. Furthermore, a quadric model was constructed efficiently. The predicted values and experimental results were close, which confirmed that the quadric model can be effectively used to predict the surface morphologies of the (Ti, Cr)ZrN films in the UBM sputtering. The experimental results were consistent with the response surface predictions. Therefore, it was concluded that the surface morphologies on multilayered films can be accurately predicted by response surface analysis, thereby justifying the reliability and feasibility of the approach.