The assessment of the elastic-plastic material behavior is imperative for benchmarking the performance of thin coating systems. Linear-elastic approaches can lead to deviating results and experimental investigations, such as fatigue tests, frequently overlook the intricacies of the failure mechanism. Therefore, the elastic-plastic material behavior of DLC based coating systems with CrN support interlayer, deposited on 100Cr6 substrates and Si, was investigated. Using an inverse approach, a nanoindentation simulation with spherical indenter geometry was iteratively optimized to experimental curves by adjusting the material parameters Young's modulus E, yield strength Y, hardening coefficient K and hardening exponent n for DLC and CrN layers. Mechanical parameters were measured and the yield strength of DLC was analyzed with a scratch procedure to implement appropriate initial values. The results showed an overall good agreement between the measured and optimized force-displacement curves with reasonable determined material parameters. The control parameter Y exhibited nearly identical outcomes for scratch measurements and the calculated value from simulations although DLC was deposited on different substrates. The employment of a spherical indenter tip mitigates the influence of the microstructure in the CrN layer through homogenization effects and a larger affected area of the plastic zone. Furthermore, enhancing the performance of the coating systems can be achieved by increasing the DLC or CrN interlayer thickness.