This paper presents a framework for guiding the design of new materials to enhance the sustainability of systems that utilize these materials throughout their production, use and retirement. Traditionally, materials engineering has focused on the interplay between material microstructure, physical properties, processing, and performance. Environmental impacts related to the system’s life cycle are not well integrated into the materials engineering process. To address this shortcoming, a new methodology has been developed that incorporates social, economic, and environmental indicators – the three dimensions of sustainability. The proposed framework accomplishes this task and provides a critical tool for use across a broad class of materials and applications. Material properties strongly shape and control sustainability performance throughout each life cycle stage including materials production, manufacturing, use and end-of-life management. Key material parameters that influence life cycle energy, emissions, and costs are highlighted. The proposed framework is demonstrated in the design of engineered cementitious composites, which are materials being developed for civil infrastructure applications including bridges, roads, pipe and buildings. This research is part of an NSF MUSES (Materials Use: Science, Engineering and Society) Biocomplexity project on sustainable concrete infrastructure materials and systems (http://sci.umich.edu).