Single-phase nanocrystalline solid solution hardened hydrogen-containing titanium zirconium carbide thin films, (Ti1-xZrx)C1-y:H, and hydrogenated nanocomposites with titanium zirconium carbide and an amorphous carbon-phase, (Ti1-xZrx)C:H/a-C:H, were deposited by reactive high power impulse magnetron sputtering. A higher degree of ionization of the molecules and sputtered atoms as well as a precise control of the thin film growth is enabled by using high power impulse magnetron sputtering. Material combinatorics was carried out by means of a systematic variation of the titanium to zirconium ratio as well as the systematic variation of the carbon content. We first used solid solution hardening for the hardness enhancement of single-phase fcc nanocrystalline (Ti1-xZrx)C1-y films. Thin film deposition was carried out by applying a segmented metallic target which consists of two pure titanium and zirconium triangle-shaped plates. The segmented target allows the realization of the material combinatorics. In this case, the deposition of 13 different titanium-to-zirconium compositions was possible in a single sputter run. With increasing the methane gas flow in the deposition process, and thereby increasing the carbon content in the film, carbon-based nanocomposites could be synthesized. Raman spectroscopy shows (Ti,Zr)C-peaks as well as the formation of an amorphous carbon phase. X-ray diffraction shows the fcc (Ti1 xZrx)C1-y phase in the single-phase and in the nanocomposites films. Elastic recoil diffraction analysis and Vickers micro-hardness were also employed in order to characterize the thin films.