Advanced materials are essential to economic security and human well-being. Accelerating the pace of discovery and deployment of advanced material systems will therefore be crucial to achieving global competitiveness in the 21st century. In 2011, US government launched the Materials Genome Initiative, a multi-agency initiative designed to create a new era of policy, resources, and infrastructure that support U.S. institutions in the effort to discover, manufacture, and deploy advanced materials twice as fast, at a fraction of the cost. Development of computational tools has been identified as one of the core components in the materials innovation infrastructure. In this talk, I will discuss how accurate and fast computational structure/property determinations can complement the traditional experimental try and error efforts in material design and discovery to accelerate the pace of technological advances. Examples from our recent studies on magnetic and battery materials will be presented. I will also discuss the challenges in bridging the gap between computational structure prediction and experimental synthesis, especially for many materials that are formed at far-from equilibrium conditions.