The isomers of gadolinium scandium mixed-metal nitride clusterfullerenes GdxSc3-xN@C(80) [x=2 (1, 4); x=1 (2, 5)] have been synthesized by the "reactive gas atmosphere" method and isolated facilely by recycling HPLC. The yield of GdxSc3-xN@C80 (I, II) (x=1, 2) relative to the homogenous clusterfullerenes Sc3N@C80 [I (3), II (6)] was determined. According to the UV/Vis/NIR spectroscopic data, 1, 2, 4, and 5 are all stable fullerenes with large optical gaps. Fullerene 1 has greater similarity to Gd3N@C80 (I) and 2 seems to resemble Sc3N@C80 (I). The quite similar overall absorption features of 4 and 5 suggest pronounced similarity in electronic structure. Vibrational spectroscopic studies led to the assignment of the cage symmetries of GdxSc3-xN@C80 (I, II), that is, Ih for 1, 2 and D5h for 4, 5. The cluster-cage interactions in GdxSc3-xN@C80 (I, II) were analyzed by means of the low-energy Raman lines. The splitting of the metal-nitrogen stretching vibrational mode in GdxSc3-xN@C80 (I, II) was studied in detail. Scalar-relativistic DFT calculations were performed to reveal the geometry parameters and the magnetic state of the GdxSc3-xN@C80 (I, II) molecules.