One of the current grand challenges in materials science and physics is the control and processing of matter away from equilibrium. This project aims to identify design rules and novel pathways to synthesize desired materials that are metastable and survive for long times at ambient conditions. This research can dramatically expand the materials design space to enable future applications – one of the goals of the Materials Genome Initiative (MGI). A motivating example is the challenge of room-temperature superconductors. That is, recently discovered high-pressure hydrides have reached the longstanding goal of room temperature superconductivity. However, they are difficult to implement in practical technologies because they decompose when they return to ambient pressure. Similar problems are encountered with other materials, such as magnets and superhard systems. In this work, metastable materials will be developed to address this critical need as they offer a promising way forward on this important front.