A new Sc-3(C-2)(CN)@I-h-C-80 metallofullerene encaging a scandium carbide/cyanide alloyed cluster was prepared and investigated. Sc-3(C-2)(CN)@I-h-C-80 was synthesized by the arc-discharging method and isolated by HPLC. Its experimental C-13 NMR spectrum with two signals clearly confirms an icosahedral C-80 cage, and theoretically calculated C-13 NMR peaks agree well with the experimental results. Further, theoretical calculations disclosed that the endohedral mu(3)-C-2 and mu(3)-CN moieties are situated on each side of the triangular shaped Sc-3 unit to form a scandium carbide/cyanide alloyed cluster. Kohn-Sham molecular orbitals reveals the electronic structure of (Sc3+)(3)(C-2)(2-)(CN)(-)@C-80(6-), in which two anions, mu(3)-C-2(2-) and mu(3)-(CN)(-), construct and stabilize this special molecule together. The FTIR and Raman spectra of Sc-3(C-2)(CN)@1(h)-C-80 were analyzed by comparison of the experimental and calculated results to further confirm its structure and to uncover cluster-based vibrational modes.