Two independent molecular structures with different bond lengths (RMSD = 0.12 Å, Table ) were observed in the asymmetric unit of [Co(1)](ClO4)2, leading us to suspect that high spin (HS) and low spin (LS) configurations co-exist in the solid state. The coordination spheres of the de novo HS and LS models of [Co(1)] 2+ each agree remarkably well, both in terms of geometry and bond lengths (RMSD = 0.05 and 0.04 Å respectively, see Table ), with one of the isomeric structures observed by SCXRD (Figure for the HS structure), supporting this proposal. Furthermore, a relatively small energetic preference for the HS configuration was predicted computationally for both the de novo structures (5.9 kJ/mol) and models of [Co(1)] 2+ derived from the corresponding SCXRD geometries (2.7 kJ/mol, see ESI for details). Predicting accurate energy gaps of multiconfigurational complexes is a challenge for DFT modelling.