Transition metal carbides, especially TaC, are particularly valued for their high thermal and mechanical stability as well as melting points of even above 4000 °C. Therefore, those materials are exceptionally interesting for the application as protective coatings. However, a considerable limitation of these materials is their high inherent brittleness. Transition metal nitrides feature lower hardness and melting points but exhibit higher fracture toughness. Inspired by the success of nano-layered superlattice architecture—shown to enhance both hardness and toughness of transition metal nitrides like TiN/CrN or TiN/WN—we prepared TiC/TaC multilayer systems via pulsed DC magnetron sputtering. By tuning bilayer periods, we determined optimum conditions for both increased hardness and improved fracture toughness. Ab initio density functional theory calculations focussing on large and small shear modulus and lattice parameter misfits suggest that carbonitride multilayer systems exhibit more ductile fracture behaviour. To investigate the influence of swapping one of the constituents of TiC/TaC with a nitride, we developed different sets of carbonitride superlattices, namely TiC/TaN and TiN/TaC. In our study we are comparing carbonitride superlattice systems consisting of the same transition metals and investigate the influence of bilayer periods and material pairings on material characteristics like mechanical, thermal and thermoelectric properties.