The synthesis of lanthanide complexes with low coordination numbers is challenging because the large ionic radii of lanthanide ions generally promote the formation of highly coordinated species. Achieving lower coordination geometries requires introducing significant steric hindrance. We report two low coordinated, almost perfectly octahedral lanthanide complexes [LnIII(Ph3PO)4(HBS)2](OTf) (Ln = DyIII (1), YbIII (2) and NdIII (3), Ph3PO = triphenylphosphine oxide; HBS = 4-hydroxybenzenesulfonate). Their magnetic and temperature-dependent luminescent properties have been systematically investigated showing field induced Single Molecule Magnet behavior and f-f optical transitions. To rationalize these properties with Complete Active Space Spin Orbit Configuration Interaction calculations, we have extended our program to compute magnetic dipole oscillator strengths. We showed that the octahedral ligand field acts as the magnetic main axes, that small geometric distortions induce significant anisotropy and simulated luminescent and magnetic data in very good agreement with experiment.