The inability of current materials to meet performance requirements is a key stumbling block for addressing grand challenges in energy and national security. Fortunately, materials research is on the brink of a new era - a transition from observation and validation of materials properties to prediction and control of materials performance. In this talk, I describe the nature of the current challenge, the prospects for success, and a specific facility concept, MaRIE, that will provide the needed capabilities to meet these challenges, especially for materials in extreme environments. MaRIE, for Matter-Radiation Interactions in Extremes, is Los Alamos' concept to realize this vision of 21st century materials research. This vision will be realized through enhancements to the current LANSCE accelerator, development of a fourth-generation x-ray light source co-located with the proton accelerator, and a comprehensive synthesis and characterization facility focused on controlling complex materials and the defect/structure link to materials performance.