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Abstract Extending the coherence lifetime of a qubit is central to the implementation and deployment of quantum technologies, particularly in the solid state where various noise sources intrinsic to the material host play a limiting role. This study examines theoretically the coherent spin dynamics of a hetero‐spin system formed by a spin featuring a non‐zero crystal field and in proximity to a paramagnetic center . An analysis of the energy level structure of the dyad shows this system exhibits apair of levels separated by a magnetic‐field‐insensitive energy gap, which can be exploited to create long‐lived zero‐quantum coherences. It is found that these coherences are selectively sensitive to “local”—as opposed to “global”—magnetic field fluctuations, suggesting these spin dyads can serve as a nanoscale gradiometer for precision magnetometry. On the other hand, the distinct response of either spin species to electric or thermal stimuli allows one to implement alternative sensing protocols for magnetic‐noise‐free electrometry and thermometry.