Endohedral metallofullerenes (EMFs) have attracted significant attention as promising spherical molecules for biomedical and material applications due to their unique properties. Endohedral metallofullerenes (EMFs), possessing a metal cluster encapsulated within the carbon cage, have demonstrated altered electronic and magnetic properties as a result of charge transfer from the metal(s) to the carbon shell, which allows a unique structure – property relationship to emerge. One family of EMFs that exhibit these unique features is the azaheterometallofullerene class containing two metals (M = Y, Gd, Tb) in a cage of 79 carbons and one nitrogen atom (M₂@C₇₉N). Our work demonstrates the importance of the azaheterometallofullerenes Gd₂@C₇₉N and Tb₂@C₇₉N as the basis for new, novel nanomaterials, such as molecular switches and single molecule magnets.