So both the spin-only susceptibility (χ s ) and the dipolar contribution to the hyperfine tensor (A dip K ) can ideally be computed using SO-CAS based methods. Fig. illustrates a comparison of the dipolar hyperfine shifts calculated from the two QC methods with the semi-classical SD (eq. S5) values based on χ s,PV of the two-KDs for the [Co(AcPyOx) 3 (BPh)] + complex. The choice to utilize only the point SD shifts, propor-tional to the spin-only ∆ χ s,PV ax due to axial symmetry (as in eq. S5), instead of the PD shifts (proportional to ∆ χ PV ax as in eq. S4) on the x-axis is to emphasize the PSO contributions considered at each level of theory. Deviation from the main diagonal line indicates the extent of PSO contributions considered with each method, subject to g-shifts and g-anisotropy. The DFT method introduces small PSO contributions, resulting in dipolar shifts mostly aligning with point SD values. Conversely, the SO-CASSCF method introduces substantial PSO shifts leading to a correlation with point SD shifts characterized by a slope close to two.