The United States’ Materials Genome Initiative (MGI), announced in 2011, helped launch the era of Materials-by-Design which combines theory, computation, experiment and data sciences to accelerate materials development and deployment. So far, Materials-by-Design research has primarily focused on the intrinsic properties of equilibrium materials. However, many technologically relevant materials are metastable and, further, roughly 1/3 or more of new materials discovered each year are metastable rather than equilibrium materials. Therefore, for new materials to help in addressing energy needs, we must directly address the research challenges of both including metastable materials and moving from Materials-by-Design to Solutions-(or Devices)-by-design. Our approach to and progress towards this challenge will be demonstrated by examples taken from current research on opto-electronic semiconductors and transparent conductors.