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The use of hybrid materials as a combination of fibre-reinforced plastic (FRP) and metal is of great interest in order to meet the increasing demands for sustainability, efficiency, and emission reduction based on the principle of lightweight design. These two components can therefore be joined using the intrinsic joining technique, which is formed by curing the matrix of the FRP component. In this study, for the hybrid joint, unidirectionally pre-impregnated semi-finished products (prepregs) with duromer matrix resin and micro-alloyed HC340LA steel were used. In order to conduct a detailed investigation, the damage mechanisms of intrinsically produced fibre metal laminates (FMLs), a new clamping device, and a novel pressing tool were designed and put into operation. The prepregs were prestressed by applying a preloading force using a specially designed prestressing frame. Hybrid specimens were then produced and subjected to nanoindentation and a shear tensile test. In particular, the effect of the residual stress state by varying the defined prestressing force on the damage mechanisms was studied. The results showed that no fracture patterns occurred in the interface of the specimens without preloading as a result of curing at 120 °C, whereas specimens with preloading failed at the boundary layer in the tensile range. Nevertheless, all specimens cured at 160 °C failed at the boundary layer in the tensile range. Furthermore, it was proven that the force and displacement of the preloaded specimens were promisingly higher than those of the unpreloaded specimens. [ABSTRACT FROM AUTHOR]