Natural materials achieve exceptional mechanical properties by relying on hierarchically structuring their internal architecture. In several marine species, layers of stiff and hard inorganic material are separated by thin compliant organic layers, giving their skeleton both stiffness and toughness. This phenomenon is fundamentally based on the periodical variation of Young’s modulus within the structure. In this study, alteration of mechanical properties is achieved through a layer-wise build-up of two different materials. A hybrid 3D-printing device combining stereolithography and inkjet printing is used for the manufacturing process. Both components used in this system, the ink for jetting and the resin for structuring by stereolithography (SLA), are acrylate-based and photo‑curable. Layers of resin and ink are solidified separately using two different light sources (λ1 = 375 nm, λ2 = 455 nm). Three composite sample groups (i.e., one hybrid material, two control groups) are built. Measurements reveal an increase in fracture toughness and elongation at break of 70% and 22%, respectively, for the hybrid material compared to the control groups. Moreover, the comparison of the two control groups shows that the effect is essentially dependent on different materials being well contained within separated layers. This bio-inspired building approach increases fracture toughness of an inherently brittle matrix material.