The reaction of di(tert-butyl)aluminum hydride with hydrazine N2H4 afforded the hydrazide (Me3C)(2)AIN(2)H(3), 1, by the release of elemental hydrogen. Compound I is a dimer ill solution and in the solid state and possesses a six-membered Al2N4 heterocycle in a twist conformation with two intact N-N bonds. Further reaction of 1 with an excess of Hal(CMe3)(2) yielded the tricyclic aluminum and nitrogen rich Al4N4 compound [(Me3C)(2)AlN2H2](2-) [Al(CMe3)(2)](2), 2, in which each N-N bond of a central six-membered Al2N4 ring similar to that of 1 is side-on-coordinated to an Al(CMe3)(2) group. The structure of 2 may be interpreted as a dimer of the dialuminum hydrazide (Me3C)(2)Al-NH-NH -Al(CMe3)(2).