A series of novel aluminum heterobimetallic selenicles were reported. The reaction of LAI(SeH)(2) (1) with LiN(SiMe3)(2) resulted in the formation of [LAI(SeLi)(2)(THF)(2)] (2) (L = HC(CMeNAr)(2), Ar = 2,6-iPr(2)C(6)H(3))- Compound 2 reacted with Me2GeCl2, Ph2GeCl2, CP2TiCl2, and CP2ZrCl2, respectively, to produce LAI(mu-Se)(2)GeMe2 (3), LAI(mu-Se)(2)GePh2 (4), LAI(mu-Se)(2)TiCP2 (5), and LAI(mu-Se)(2)ZrCp2 (6) in moderate yields. Compounds 2-6 were characterized by elemental analysis, NMR, and electron impact-MS. The X-ray single-crystal structure of 3 is reported and confirms the spirocyclic arrangement of the aluminum atom within the six-membered AlN2C3 and four-membered AlSe2Ge rings.