Y-2@C79N and Tb-2@C79N have been prepared by conducting the Kratschmer-Huffman electric-arc process under 20 Torr of N-2 and 280 Torr of He with metal oxide-doped graphite rods. These new heterofullerenes were separated from the resulting mixture of empty cage fullerenes and endohedral fullerenes by chemical separation and a two-stage chromatographic process. Crystallographic data for Tb-2@C79N-Ni(OEP)center dot 2C(6)H(6) demonstrate the presence of an 80-atom cage with idealized I-h symmetry and two, widely separated Tb atoms inside with a Tb-Tb separation of 3.9020(10) A for the major terbium sites. The EPR spectrum of the odd-electron Y-2@C79N indicates that the spin density largely resides on the two equivalent yttrium ions. Computational studies on Y-2@C79N suggest that the nitrogen atom resides at a 665 ring junction in the equator on the fullerene cage and that the unpaired electron is localized in a bonding orbital between the two yttrium ions of this stable radical. Thus, the Tb-Tb bond length of the single-electron bond is an exceedingly long metal-metal bond.