Several studies have revealed the sensitivity of the SCO behavior to minute structural changes in the immediate surrounding of the central metal ion. DFT and a model Hamiltonian approach, for example, established the connection between the pressure-dependent iron-nitrogen distances and the SCO process in a dinuclear Fe(II) complex. The observation that magnetic properties are very sensitive to small structural changes has been made in a mixed experimental/DFT study on Co(SPh) 4 (PPh 4 ) 2 , a single-molecule magnet. Moreover, in an investigation using Monte Carlo simulation techniques, the coupling between SCO centers was described as harmonic stretching and bending interactions, highlighting the importance of geometric and vibronic effects in SCO complexes. These examples demonstrate that, while the computational modeling of (pressure-induced) SCO is a highly challenging endeavor, several examples prove that today's simulation methods can be used to gain both fundamental and practical insights into SCO processes. Further methodological advancements in the underlying electronic structure theory as well as the development of multiscale simulation approaches will surely continue to contribute to our understanding of SCO processes at the molecular level.