Since the millenium-old invention of steel, innovative materials that may withstand extreme conditions of high loads, heat and/or irradiation represent key drivers of industrial and technological progress. Recently, the focus has been set on concentrated, multicomponent alloys, that may not only provide excellent mechanical properties, but also may reduce overall costs and weight. However, this search of novel materials requires high throughput measurements and multiscale modeling predictions that may help navigate through the multidimensional composition space. Such “materials informatics” may be performed either “top-down”, by starting from experimental outcomes, or “bottom-up”, by starting from fundamental principles. In this presentation, I will describe efforts and accomplishments across both informatics routes, by describing work on digital image correlation, nanoindentation, and electron microscopy data, but also present progress on composition search criteria built upon crystal dislocation features, and electron charge profiles.