Enabling the rational synthesis of molecular candidates for quantum information processing requires design principles that minimize electron spin decoherence. Here we report a systematic investigation of decoherence via the synthesis of two series of paramagnetic coordination complexes. These complexes, [M(C2O4)(3)](3-) (M = Ru, Cr, Fe) and [M(CN)(6)](3-) (M = Fe, Ru, Os), were prepared and interrogated by pulsed electron paramagnetic resonance (EPR) spectroscopy to assess quantitatively the influence of the magnitude of spin (S = 1/2, 3/2, 5/2) and spin orbit coupling (zeta = 464, 880, 3100 cm(-1)) on quantum decoherence. Coherence times (T-2) were collected via Hahn echo experiments and revealed a small dependence on the two variables studied, demonstrating that the magnitudes of spin and spin-orbit coupling are not the primary drivers of electron spin decoherence. On the basis of these conclusions, a proof-of-concept molecule, [Ru(C2O4)(3)](3-), was selected for further study. The two parameters establishing the viability of a qubit are a long coherence time, T-2, and the presence of Rabi oscillations. The complex [Ru(C2O4)(3)](3-) exhibits both a coherence time of T-2 = 3.4 mu s and the rarely observed Rabi oscillations. These two features establish [Ru(C2O4)(3)](3-) as a molecular qubit candidate and mark the viability of coordination complexes as qubit platforms. Our results illustrate that the design of qubit candidates can be achieved with a wide range of paramagnetic ions and spin states while preserving a long-lived coherence.