The convergence of new computational capabilities, advanced characterization techniques and the ability to generate and use large-scale data provides new opportunities for rapid development and deployment of advanced materials. These opportunities have recently been recognized by the National Materials Genome Initiative (MGI). Ideally, a predictive computational infrastructure that permits (a) materials design by passing information “up” the length-scales from the atomic scale to the mesoscale as well as (b) engineering component design by the inverse passing of information “down” the scales is needed. Considering the critical need for calibration and validation of computational models, new tools for rapid characterization of material structure and properties are also needed, along with platforms for capturing, managing and analyzing large, multimodal datasets. Examples of computational and experimental tools that are accelerating the development of new structural and functional materials will be discussed along with major challenges that remain.