Strategy (iv) of using ligands that are simultaneously strong σ and π-donors such as the phenyl-anion appears to be successful, as large ∆E LFS close to the of VCl 3 (ddpd) is found for several complexes (5, 9, 13, 15) and even larger ∆E LFS is found for [VCl 3 (py-ph-py)] -( ) and [VCl 3 (im-ph-im)] - (12). Among the phenyl-anion-bearing complexes, the smallest ∆E LFS is found for 14, 16, and 17 with 2, 3, and 3 phenyl-anion groups, respectively, indicating that a too large number of phenyl-anion ligands can be detrimental for large ligand-field splitting. A previous computational study predicted for bis-tridentate iron(II) complexes that triplet metal-centered states are stabilized -hinting to a smaller ligand-field splitting -when the phenyl-anion ligands constitute the central part of the tridentate ligands, while the states are destabilized when the phenyl-anion is in one of the peripheral positions. Our screening does not find this trend repeated for vanadium(III) complexes, as we observe the largest ligand-field splitting indeed when the phenyl-anion assumes the central position of the tridentate ligand, e.g., as in [VCl 3 (py-ph-py)] -or [VCl 3 (im-ph-im)] -. Finally, strategy (v) of using stronger-field monodentate ligands from the spectrochemical series in place of the Cl -ligands appears to be detrimental to achieve large ligandfield splitting. Using the strong-field monodentate NO - 2 and CO ligands decreases ∆E LFS considerably (1, 6), while using the OH - ligand which is more similar in strength to the Cl -ligand yields also a similar ∆E LFS in complex 2.