Metallic (M) and polymer (P) materials as layered hybrid metal-polymer-metal (MPM) sandwiches offer a wide range of applications by combining the advantages of both material classes. The interfaces between the materials have a considerable impact on the resulting mechanical properties of the composite and its structural performance. Besides the fact that the experimental methods to determine the properties of the single constituents are well established, the characterization of interface failure behavior between dissimilar materials is very challenging. In this study, a mixed numerical–experimental approach for the determination of the mode I energy release rate is investi-gated. Using the example of an interface between a steel (St) and a thermoplastic polyolefin (PP/PE), the process of specimen development, experimental parameter determination, and numerical calibration is presented. A modified design of the Double Cantilever Beam (DCB) is utilized to characterize the interlaminar properties and a tailored experimental setup is presented. For this, an inverse calibration method is used by employing numerical studies using cohesive elements and the explicit solver of LS-DYNA based on the force-displacement and crack propagation results.