Magnetron sputtering is a powerful process for the production of thin films and coatings employed for the surface modification of tools and engineering components in various industrial sectors. Nanostructured coatings for multifunctional applications were deposited by means of magnetron sputtering by adjusting the experimental parameters in order to tailor the chemistry, the microstructure and the morphology of the coatings. Among the several systems that were investigated, TiC–TiB2 for wear applications were successfully tested. TiC–TiB2 coatings were deposited on a hardmetal WC–Co substrate in an unbalanced DC magnetron sputtering system starting from composite targets fabricated by the Self-propagating High-temperature Synthesis (SHS) consolidation method, involving the material synthesis and densification in one step. The results, showing the achievement of nanostructured films with thickness ranging between 1 and 2 µm, are here presented. The properties evaluated on the developed films (hardness, adhesion, friction coefficient and volumetric wear) are promising for the improvement of wear-resistant applications.