Diamond-like carbon (DLC) films have attracted great interest due to their outstanding mechanical, biocompatibility, thermal, optical and electrical properties. The DLC films can be produced by microwave plasma chemical vapor deposition (MPCVD) using Argon, methane and hydrogen mixed gases. The film properties depend strongly on the experimental parameters such as substrate temperatures; microwave power, process pressure and hydrogen concentration (H2/Ar+CH4+H2). In this study, the properties of nanomechanics of DLC films with various experimental parameters are firstly discussed which include hardness and Young’s modulus characterizing by depth-sensing nanoindentation technique. The nanoindentation is an excellent method for measuring nanomechanical properties of both bulk and thin films. The probe was conducted using a Berkovich diamond tip. To find the optimized process parameters, the statistical and mathematical response surface methodology (RSM) is used to model and analyze the effect of substrate temperature (T), microwave power (W), process pressure (P) and hydrogen concentration (H) on the properties of nanomechanics of DLC films. The central composite experimental design (CCD) is used to evaluate the interaction parametric effects of multiple experimental variables on process response (hardness and Young’s modulus). The predictive quadratic model proposed herein considering the analysis of variance (ANOVA) are proved to fit and predict values of the hardness and Young’s modulus close to those readings recorded experimentally. The most significant influential factors for maximizing the hardness and Young’s modulus have been identified from the ANOVA table. The RSM technique is demonstrated to be a powerful tool in exploration of the manufacturing parameters space of complex physical process of DLC films deposition by MPCVD.