Dy … Cp R centroid angle approaches linearity. Calculations on relatively small dysprosocenium cations like [Dy(Cp*)2] + (Cp* = C5Me5) predict very slow Orbach relaxation, due to limited vibrations that are off-resonance with electronic transitions. However, due to predominantly electrostatic Ln bonding regimes, the reduced ligand steric bulk of Cp* allows significant equatorial interactions with weakly coordinating anions (WCAs) and donor solvents; these promote magnetic relaxation and reduce magnetic hysteresis temperatures (TH) compared to isolated dysprosocenium cations (which have reached up to 80 K). As the multistep syntheses of air-and moisture-sensitive target molecules can be arduous, we envisaged that in silico screening could provide a more efficient approach to identify isolable dysprosocenium cations in advance of laboratory work. Datasets and programs that can be used to make systematic predictions of the effect of ligand steric bulk on metal coordination spheres include the Tolman cone angle, Solid-G, and (minimum) percent buried volume, %Vbur(min); however, these approaches do not consider if ligands or substituents may act in concert to prevent coordination.