In this work, DFT calculations are performed in order to provide a basis for the assemblage of Gd-based supramolecular magnetic hyperalkali complexes that combine strong donor character and outstanding magnetic response. When the Gd atom is decorated with the lithiated superalkali moieties Li3O and Li4O, the calculated vertical ionization potential (VIP) is observed to drop to 3.75 eV for the Gd(Li3O)(4) cluster, and 3.58 eV for the Gd(Li4O)(3) cluster, which are below the VIP of cesium (3.99 eV) calculated at the same level of theory. A recipe earlier proposed for obtaining hyperalkali molecules is verified. By using the hypermetalated cluster Li4O in number that matches exactly the formal valence of Gd, we observe the lowest VIP, where the next excess electron provides the enhancement of the donor character besides stabilizing the cluster. The results indicate a new concept for designing highly reactive molecules.