The influence of the chemical composition of Co-based metallic glasses on the electronic structure, topology, stiffness and fracture toughness is investigated. The material selection for the experiments is based on our ab initio MD data. For efficient investigation a physical vapour deposition combinatorial approach will be applied. Selected metallic glass compositions will be grown in the bulk form to further characterize relevant mechanical properties, such as fracture toughness. Topological and chemical ordering is analysed by atom probe tomography, selected area electron diffraction with a transmission electron microscope and high energy XRD techniques. It is envisioned that based on this research strategy the basic physical and chemical design principles required to realize future knowledge-based design of metallic glasses with high strength and stiffness as well as toughness can be identified.