Summarizing we find that strategies (i) and (iv) of including strong σ donors or σ /π donors are the most promising in finding complexes with larger ligand-field splitting compared to the usage of π-acceptor ligands as in strategy (iii). Strategy (ii) of aiming for higher symmetry in the complexes appears to have only a small influence on ∆E LFS , while strategy (v) of using stronger-field monodentate ligands proved to be detrimental for large ligand-field splitting in the tested vanadium(III) complexes.