Development of optimized hard coatings requires a multilayer, functionally gradient approach, where adhesion, load support and low friction regions must be elements of the design architecture. Each of these functional regions should be joined through appropriate transition regions to reach desired coating performance. The design of coatings with hard and lubricious diamond-like carbon (DLC) surfaces requires a study of transitions between adhesive metal, load supporting carbide, and wear-resistant DLC materials. These transitions were investigated on the Ti-C system prepared by a hybrid of magnetron sputtering and pulsed laser deposition. Crystalline alpha-Ti, TiC and amorphous DLC films were formed at 100 degrees C substrate temperature by varying film chemical composition. Phase transitions between Ti-TiC-DLC were analyzed with XPS, XRD and Raman spectroscopy. A gradual replacement of hcp alpha-Ti with fee TiC, and a two-phase region consisting of crystalline TIC and amorphous carbon (a-C) in transitions from Ti to TiC and from TiC to DLC were found. These transitions were reflected in mechanical properties investigated with nanoindentation. A hardness maximum in the two-phase TiC/a-C region was found. The resulting composition-property maps were used to design a wear-resistant coating with Ti/TiC/DLC transitions and a gradual increase in hardness from a steel substrate to a super-hard (60-70 GPa) self-lubricating DLC layer on the surface. This provided a hard coating with a low friction surface, which also resisted brittle failure in tests with high contact loads.