The dimeric iminoalane, [CpAlN(2,6-i-Pr2C6H3)](2) (2), has been prepared from a double dealkylation reaction between Cp(3)Al and 2,6-diisopropylaniline. The single-crystal X-ray structure of 2 reveals a nearly square planar Al2N2 Core, with each cyclopentadienyl ring coordinated to its aluminum atom in a pentahapto fashion. This structure represents the first solid-state characterization of an eta(5)-coordination geometry between a simple C5H5 ring and aluminum.