Quantum information processing (QIP) could revolutionize areas ranging from chemical modeling to cryptography. One key figure of merit for the smallest unit for QIP, the qubit, is the coherence time (<i>T</i><sub>2</sub>), which establishes the lifetime for the qubit. Transition metal complexes offer tremendous potential as tunable qubits, yet their development is hampered by the absence of synthetic design principles to achieve a long <i>T</i><sub>2</sub>. We harnessed molecular design to create a series of qubits, (Ph<sub>4</sub>P)<sub>2</sub>[V(C<sub>8</sub>S<sub>8</sub>)<sub>3</sub>] (<b>1</b>), (Ph<sub>4</sub>P)<sub>2</sub>[V(β-C<sub>3</sub>S<sub>5</sub>)<sub>3</sub>] (<b>2</b>), (Ph<sub>4</sub>P)<sub>2</sub>[V(α-C<sub>3</sub>S<sub>5</sub>)<sub>3</sub>] (<b>3</b>), and (Ph<sub>4</sub>P)<sub>2</sub>[V(C<sub>3</sub>S<sub>4</sub>O)<sub>3</sub>] (<b>4</b>), with <i>T</i><sub>2</sub>s of 1–4 μs at 80 K in protiated and deuterated environments. Crucially, through chemical tuning of nuclear spin content in the vanadium(IV) environment we realized a <i>T</i><sub>2</sub> of ∼1 ms for the species (<i>d</i><sub>20</sub>-Ph<sub>4</sub>P)<sub>2</sub>[V(C<sub>8</sub>S<sub>8</sub>)<sub>3</sub>] (<b>1</b>′) in CS<sub>2</sub>, a value that surpasses the coordination complex record by an order of magnitude. This value even eclipses some prominent solid-state qubits. Electrochemical and continuous wave electron paramagnetic resonance (EPR) data reveal variation in the electronic influence of the ligands on the metal ion across <b>1</b>–<b>4</b>. However, pulsed measurements indicate that the most important influence on decoherence is nuclear spins in the protiated and deuterated solvents utilized herein. Our results illuminate a path forward in synthetic design principles, which should unite CS<sub>2</sub> solubility with nuclear spin free ligand fields to develop a new generation of molecular qubits