Analysis of experimentally characterized SCOs allowed us to extract experimental transition temperatures directly from the manuscript. Comparison of computationally predicted T1/2 to experimentally reported T1/2 revealed that while T1/2 predictions from modB3LYP (aHF = 0.10), M06-L, and TPSSh show limited correlation to experimental T1/2, they are largely consistent among the three DFAs. Thus, while these three DFAs predict SCO behavior for most complexes, they do not necessarily predict the same relative SCO temperatures as experiment. We also identified the reasons for the largest disagreement of DFT predictions of SCO behavior with experiments to be the lack of counter-anions and crystal packing effects in the DFT calculations, as well as the lack of packing effects to predict phenomena like hysteresis and two-step SCO behavior.