PVD coatings with high wear resistance are commonly applied to protect cutting tools from wear under high thermomechanical loads during cutting processes. In this study, the influence of cobalt content in cemented carbide (WC/Co) substrates and the interlayer thickness in a TiAlCrN coating system on tool wear and thermomechanical load is investigated. TiAlCrN PVD coatings with three different interlayer thicknesses were applied to WC/Co substrates with two different Co contents. The coating properties of these six coating-substrate systems were first determined. The coated cutting tools were then subjected to turning experiments to evaluate tool wear of the six coating-substrate systems. Using coating properties and the collected data from the cutting experiments, the thermomechanical load of the tool was simulated by means of finite element (FE) simulation. The simulation shows that the stresses in the tool are higher with increased Co content. The simulation results align with the findings from the turning experiments and will be used in further studies as a whitebox-model (FE simulation) in a greybox approach (model combining FE simulation and data-driven machine learning method).