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The nitrogen-vacancy (NV) center in diamond, a well-studied, optically active spin defect, is the prototypical system in many state-of-the-art quantum sensing and communication applications. In addition to the enticing properties intrinsic to the NV center, its diamond host's nuclear and electronic spin baths can be leveraged as resources for quantum information rather than considered solely as sources of decoherence. However, current synthesis approaches result in stochastic defect spin positions, reducing the technology's potential for deterministic control and yield of NV spin bath systems, as well as scalability and integration with other technologies. Here, we demonstrate the use of theoretical calculations of electronic central spin decoherence as an integral part of an NV spin bath synthesis workflow, providing a path forward for the quantitative design of NV center-based quantum sensing systems. We use …