Optically active spin defects in the solid-state are key for applications in quantum information science, quantum sensing, and quantum networks. In particular, the neutral divacancy (VV0) defect in silicon carbide (SiC) can be leveraged for these applications because it boasts long coherence times, a robust spin-photon interface, and the added benefit of being hosted in a technologically mature semiconductor. Additionally, nuclear spins inherent in the material provide a key resource for local quantum memories due to their long coherence times. In this thesis, we demonstrate that in isotopically purified material VV0 qubits display record-long coherence times of individual electron and nuclear spins, single shot readout of the electron and nuclear spin states, and in-situ device tunability of the electron’s optical and spin properties. Ultimately, these findings harness the synergy between materials growth and device integration to create a highly coherent solid-state quantum node. This thesis focuses on how we achieve single-shot readout of VV0, enabling long spin coherences time measurements in isotopically purified material. We then integrate a VV0 center in a p-i-n diode, a scalable classical electronic device, with isotopically purified material in the intrinsic region to tune the optical and spin properties of the VV0. Using dynamical decoupling sequences in these isotopically purified materials, we first measure single electron spin T2 > 5 s and then couple the electron spin in the diode device to a single nuclear register nearby to record its minutes-long coherence. Overall, this thesis develops VV0 spins for quantum technologies that require a tunable quantum interface and explores the understanding of magnetic and electronic noise on the spins in the material.