Nanoindentation, i.e., the probing of a material’s response when penetrating its surface at the nanometer scale with a sharp tip of defined shape, has recently emerged as an important technique for locally characterizing mechanical properties. Although its initial applications were geared towards thin films, nanoindenters have evolved into a versatile characterization tool capable of obtaining information that is difficult or impossible to access with traditional methods such as high- and low-temperature testing, high strain rate testing, creep testing, etc. In our research, we perform nanoindentations using both standard commercial instrumentation as well as, for resolution down to the atomic scale, atomic force microscopes to analyze the mechanical properties of bulk metallic glasses (BMGs) and metal alloys sputtered as thin films on silicon wafers using a combinatorial approach. While the research on the bulk samples is designed to provide insight into the plastic flow properties of such glasses, which are currently not conclusively known, the wafer studies are aimed at unveiling the complex correlations between materials properties and an alloy’s glass forming ability in order to extract trends that will allow to dramatically accelerate the development of multi-component alloys with tailored properties.