Establishing systems-based materials design methods is an important step towards enabling rapid, concurrent design of materials and products with the potential for significant technological innovations. Materials design involves tailoring material structures and processing paths to achieve properties and performance levels that are customized for a particular application. It is a complex, non-deterministic, multi-scale, multifunctional activity that requires multiple collaborating designers and distributed, heterogeneous computing resources. Accordingly, a systems-based design approach is required with which to manage information flows, embed performance-property-structure-processing relations, interrogate models, explore variability, and engage collaborative decision-support protocols. In this paper, we discuss some of the intellectual and computing foundations of our systemsbased approach for materials design. It has three primary facets: (1) a decision support framework for modeling and supporting a complex, collaborative design process, (2) robust design methods for modeling uncertainty and managing or minimizing its impact on design specifications, and (3) a computational infrastructure for integrating and sharing heterogeneous information and computing and software resources. Some of the key aspects of our approach are illustrated via design of multifunctional cellular materials for a structural heat exchanger application.