The recognition and in-depth understanding of inverse trans influence (ITT) have successfully guided the synthesis of novel actinide complexes and enriched actinide chemistry. Those complexes, however, are mainly limited to the involvement of high-valence actinide and/or metal-ligand multiple bonds. Examples containing both low oxidation state actinide and metal-metal single bond remain rare. Herein, more than 20 actinide-transition metal (An-TM) complexes of phosphinoaryl oxide ligands have been designed in accordance with several experimentally known analogs, by changing the metal atoms (An = Th, Pa, U, Np, and Pu; and TM = Ni, Pd, and Pt), actinide oxidation states (IV and III) and metal-metal axial donor ligands (X = Me3SiO, F, Cl, Br, and I). The relativistic density functional theory study of structural (trans-An-X and cis-An-O toward An-TM), bonding (topological electron/energy density), and electronic properties reveals the order of the ITI stabilizing actinide-metal bond. Computed electron affinity (EA) values, related to the electrochemical reduction, linearly correlate with experimentally measured reduction potentials. Although the same ITI order for the ligand donors was shown as in a previous study, the correlation between electrochemical reduction and the ITI was found to be weak when the actinide atoms were changed. For most complexes, the reduction is primarily of an actinide-based mechanism with minor participation of transition metal and phosphinoaryl oxide, whereas that of thorium-nickel complexes is different.