This collaborative effort parallels goals of the Materials Genome Initiative. Concepts and methods for predictive materials discovery will be developed in the context of theory-driven design of polypeptides that assemble into targeted materials and nanostructures. New experimental methods for studying and guiding molecular assembly in solution will be refined to monitor polypeptide assembly and to build polypeptide/nanoparticle materials with hierarchical complexity. The close interaction of theory and experiment is essential in the development of a predictive understanding of these materials. The concepts and methods so developed will speed the discovery of new polypeptide-based hybrid materials, and the use of the peptides to specify the arrangement and positioning of metal nanoparticles, has a variety of potential applications, including enhancement of light capture in photovoltaic cells.