The High-Throughput Experimental Materials Collaboratory (HTE-MC) is a federated network of integrated materials synthesis‒characterization‒data management services designed to rapidly generate large volumes of high-quality experimental data to significantly improve predictive design in materials science. The HTE-MC vision is (1) building a sustainable ecosystem of resources to empower innovators, (2) fostering standards and best practices, and (3) incorporating artificial intelligence to enable game-changing scientific and technological breakthrough. Numerous recent reports have identified opportunities and gaps at the intersection of high-throughput experimentation, materials data infrastructure, and materials informatics. We propose to focus on High Entropy Alloys (HEA) as the first major use case for the HTE-MC, due to their unique properties and critical high technology applications. The HTE-MC will enable participation among industry, government, and academia, and drive creation of a next-generation workforce while enabling the creation of new materials and products.