Dedicated to Professor Philipp GütlichRecently the oligomeric and polyhedral compounds of aluminum containing Al À N and Al À C cores have attracted considerable interest following the preparation of a few threecoordinate iminoalanes [1] and the determination of the structures of carbaalanes. [2] Heteroatom-containing organoaluminum cage compounds [3] are potential precursors for various applications such as catalysts, reagents, and for chemical vapor deposition, [3a, 4, 5] as well as being of theoretical importance. [6] Although the formation of iminoalanes and carbaalanes is now almost understood, [1±3] compounds containing an Al n C n N n framework (n b 2) are still unknown. [7] We figured that such species should exhibit some interesting features. Herein we report the structure of the polyhedron 1 and the synthesis of the bridging compound with bulky pyrazolato ligands 2 (tBu 2 pz 3,5-di-tert-butylpyrazolato).