This thesis describes studies on atomic point defects in semiconductors for applications in quantum information. In particular, its focus is on defects whose energy levels reside deep within the bandgap certain semiconductors because these systems can behave like artificial trapped atoms in the solid state, possessing optical addressability, long coherence times, and the ability to be manipulated at microwave frequencies. The most prominent defect in this field of study is the diamond nitrogen-vacancy center, whose functionality is well-known to persist to ambient temperature. The first part of this thesis investigates the persistence of this functionality to temperatures upwards of 600 K. Importantly, these investigations also demonstrate that the diamond nitrogen-vacancy center can be a sensitive thermometer (~10 mK/Hz^(1/2)) over a wide range of temperatures with nanoscale spatial resolution. The latter part of the thesis describes experimental measurements of divacancy defects in silicon carbide, a potential alternative materials host to diamond with established wafer-scale growth and microfabrication capabilities. Single divacancy spins are isolated and coherently controlled for the first time in the 4H polytype of silicon carbide, and the divacancy's coherence is shown to be a remarkably long T2 = 1.2 ms at T = 20 K. The last chapter extends these results by isolating single divacancies in the 3C polytype, experimentally demonstrating a qualitative and quantitative model of their spin and orbital dynamics, and revealing the divacancy's excited state level structure in both the 3C and 4H polytypes using resonant laser techniques. These excited state transitions are shown to posses a structure identical to the diamond nitrogen-vacancy center and a subset are shown to have favorable cycling properties. The location of a clear spin-photon interface has important implications for high-fidelity quantum state readout and photon-based entanglement schemes that use divacancy spins.