A series of novel organozinc aminoalcoholates have been synthesized by the reaction of the amino alcohols HOCHx(CH2NMe2)(3-x) (x = 2, Hdmae; 1, Hbdmap; 0, Htdmap) with R2Zn (R = Me, Et). The 1:1 reaction with Hdmae leads to the tetramers [RZn(dmae)](4) [R = Me (1), Et (2)], while with Htdmap, dimeric [RZn(tdmap)](2) [R = Me (7), Et (8)] are produced. Reaction with Hbdmap only yields [MeZn(bdmap)](n) (3), an oil which mass spectral data suggests contains a mixture of Zn-2 - Zn-7 species, when a 2-fold excess of ligand is used. Crystals of dimeric [Zn(bdmap)(2)center dot Hbdmap](2) (4) deposit from this oil on prolonged standing. Reaction of Et2Zn with Hbdmap (1:1) affords [EtZn(bdmap)](n) (5), also an oil made up of Zn-3 and Zn-4 clusters on the basis of mass spectral evidence. Crystals of EtZn3(bdmap)(5) (6) are formed within the oil that is 5 on standing. [MeZn(tdmap)](2) (7) has been used as a single-source precursor for hexagonal ZnO films under low pressure chemical vapor deposition (LPCVD) conditions and a substrate temperature of 500 degrees C.