The past decade has seen remarkable progress in the development of the nitrogen-vacancy (NV) defect center in diamond, which is one of the leading candidates for quantum information technologies. The success of the NV center as a solid-state qubit has stimulated an active search for similar defect spins in other technologically important and mature semiconductors, such as silicon carbide. If successfully combined with the advanced microfabrication techniques available to such materials, coherent quantum control of defect spins could potentially lead to semiconductor-based, wafer-scale quantum technologies that make use of exotic quantum mechanical phenomena like entanglement. In this article, we describe the robust spin property of the NV center and the current status of NV center research for quantum information technologies. We then outline first-principles computational modeling techniques based on density functional theory to efficiently search for potential spin defects in nondiamond hosts suitable for quantum information applications. The combination of computational modeling and experimentation has proven invaluable in this area, and we describe the successful interplay between theory and experiment achieved with the divacancy spin qubit in silicon carbide.