The development of combinatorial synthesis methods such as combinatorial co-deposition of thin-film materials libraries opens new perspectives for cost-effective and efficient searching of novel materials with attractive properties or even unusual features. The main advantage of this approach is that in a single process, hundreds or even thousands of alloys can be produced. Combining combinatorial synthesis methods with high-throughput characterization techniques, e.g. automatic chemical analysis and phase analysis with programmable sample-positioning stages, high-speed nanoindentation, etc., allows for the fast screening of a wide range of compositions and correlation with desired mechanical, optical, magnetic, etc. properties. In the present work, we performed a series of systematic experiments to investigate the microstructure and mechanical properties of the CoCr material library, synthesized via magnetron co-sputtering, in a wide compositional range. We focused on the correlation of the phase composition and texture with mechanical properties to extract the dominant factors influencing the strength of the nanocrystalline (nc) CoCr system. In the investigated part of the nc CoCr system, a relatively broad spectrum of compressive yield strength was found i.e. from 1.41 GPa for the as-deposited CoCr36 alloy up to 3.64 GPa for the annealed CoCr66 alloy and they partially go beyond the box of regular alloys properties in the Ashby map for the given density class. The findings of this study are transferable to other systems and can be used to optimize the strategy of high-throughput searching for materials with exceptional properties.