The inherent atomic level structural control of synthetic chemistry enables the creation of qubits, the base units of a quantum information science system, designed for a target application. For quantum sensing applications, enabling optical read-out of spin in tunable molecular systems, akin to defect-based systems, would be transformative. This approach would bring together molecular tunability with optical read-out technology. In theory, nickel ions in octahedral symmetry meet all the criteria for optical readout of spin. Yet, to the best of our knowledge, there are no pulse EPR studies on Ni2+ molecules. We identified two compounds featuring highly symmetric Ni2+ centers, thereby engendering weak zero-field splitting to enable EPR addressability: [Ni(phen)3](BF4)2 (1) and [Ni(pyr3)2](BF4)2 (2) (phen = 1,10-phenanthroline; pyr3 = tris-2-pyridyl-methane). Crucially, these complexes feature the requisite strong field ligands to enable emission for optical addressability. We extracted axial zero-field splitting parameters of D = +0.9 cm-1 and +2.7 cm-1 for 1 and 2, respectively, enabling pulse EPR measurements. Both compounds produce emission at λmax = 938-944 nm. The aggregate of these results expands the catalogue of qubit materials to Ni2+-based compounds and offers a future pathway for optical readout of these molecules.