The novel methylcadmium aminoalkoxides MeCd(dmae) (Hdmae = dimethylaminoethanol), MeCd(bdmap) [Hbdmap = 1,3-bis-(dimethylamino)-propan-2-ol], and MeCd(tdmap) [tdmap = 1,3-bis(dimethylamino)-2-(dimethylaminomethyl)propan-2-ol] have been synthesized and structurally characterized. MeCd(dmae) (1) forms a tetrameric heterocubane with a Cd4O4 core, while MeCd(bdmap) (2) is trimeric and MeCd(tdmap) (3) is a dimer. Only in the case of MeCd(dmae) are all the ligand donors fully utilized. In solution, MeCd(tdmap) undergoes a Schlenk equilibrium, with Me2Cd and Cd(tdmap)(2) evident at 218 K. The structure and solution-state chemistry of Cd(tdmap)(2) (5) have been independently studied and, in the solid-state, found to exist as a dimer whose coordination number at cadmium (CN = 6) is greater than in the organocadmium complexes (CN = 4, 5). MeCd(tdmap) has been used as a single-source precursor for CdO films by LPCVD with a glass substrate temperature of only 140 degrees C. Evidence is also presented for the formation of a heterometallic precursor, [(MeZn)(MeCd)(tdmap)(2)] (6), which has been used to deposit films of CdO mixed with ZnO by LPCVD at 140 degrees C. The structure of Me4Cd4(tdmap)(2)Cl-2 (4), obtained serendipitously, is also included. Crystal data: 1, C20H52Cd4N4O4, FW 862,26, triclinic, P (1) over bar, a = 11.47560(10), b = 13.55400(10), c = 21.5966(2) angstrom, alpha = 99.7869(4), beta = 90.7476(4), gamma = 98.7823(4)degrees, V = 3268.82(5) angstrom(3), Z = 4; 2, C27H67Cd3N6O3, FW 861.07, triclinic, P (1) over bar, a = 11.4148(2), b = 13.1886(2), c = 14.3139(3) A, alpha = 102.1962(10), beta = 108.3064(10), gamma = 100.8446(10)degrees, V = 1923.09(6) angstrom(3), Z = 4; 3, C22H54Cd2N6O2, FW 659.51, monoclinic, P2(t)/n, a = 10.2912(1), b = 13.46930(1), c = 11.79130(1) angstrom, beta = 112.8051 (1)degrees, V = 1506.59(2) angstrom(3), Z = 2; 4, C24H60Cd4Cl2N6O2, FW 985.28, monoclinic, P2(1)/c, a = 10.89780(10), b = 20.3529(2), c = 16.5317(2) A, p = 94,8550(10)degrees, V = 3653.61(7) angstrom(3), Z = 4; 5, C40H96Cd2N12O4, FW 1034.09, orthorhombic, P2(1)cn, a = 12.33290(10), b = 14.25060(10), c = 29.9003(2) angstrom, V = 5255.01(7) angstrom(3), Z = 4.