Experimental results on two supramolecular complexes in which a Cr III or Fe III d-orbital single-ion magnet center is embedded between a pair of Fe II spin-crossover moieties make those two complexes interesting as possible candidates for use in quantum information technologies. We report detailed computational results for their structure and electronic properties and use the resulting data to parametrize a spin Hamiltonian that facilitates comparison with experimental results and their interpretation. Consistent with experimental results on decoherence in [Fe(ox) 3 ] @[Fe 2 L 3 ] + , we find it to be easy-plane type while the [Cr(ox) 3 ] @[Fe 2 L 3 ] + system is easy-axis type.