Point defects in wide-bandgap semiconductors have emerged as leading platforms for quantum information science and technology, because they host isolated electron and nuclear spin states that can be addressed optically and electronically for use as qubits and quantum sensors. However, most research to date has concentrated on only a few defect systems and host materials, and the identification of new defect systems has been a slow, arduous, and generally ad hoc process. Given the vast number of potential materials and defect configurations, it remains a major challenge to theoretically predict and experimentally identify promising candidates in a systematic way. This collaborative DMREF project will address this challenge by combining new computational and experimental techniques to accelerate the discovery of defects, dopants, and host materials optimized for spin-light quantum interfaces. Computationally efficient analytic group theory-based models supported by judicious use of ab initio and low-energy numerical calculations will facilitate the systematic discovery of electronic systems with desired properties, while novel high-throughput single-emitter spectroscopy techniques will enable rapid experimental characterization. The immediate goal of the project is to identify previously unexplored spin systems that support coherent spin-photon interfaces at or near room temperature, using state-of-the art techniques for quantum dynamical control. More broadly, the ability to select defects that satisfy particular materials and application requirements will revolutionize solid-state quantum engineering and lead to diverse new applications of quantum science.