The electronic structures of 3-Dy•C6H6 and 4-Dy were investigated by CASSCF-SO calculations using OpenMolcas 66 and the atomic coordinates from SCXRD datasets (See ESI for details). In both complexes the ground state principal magnetic axis (gz) traverses the two Cp R , and the axiality of each ground doublet is confirmed by both their Ising-like g values (gx ~ gy ~ 0, gz = 19.9) and dominant mJ = ±15/2 character 3-Dy•C6H6 (99.6%) and 4-Dy (99.4%).