Reaction of Me3M (M = Al, Ga) with 1-aminoadamantane, Ada, in toluene affords crystalline complexes of the type [Me2M-Ada]2. The gallium compound, I, isomorphous with the aluminum compound, II, crystallizes in the triclinic space group P1BAR with unit cell parameters a = 6.728(1), b = 9.957(2), c = 10.341(2) angstrom, alpha = 74.30(1), beta = 73.94(1), gamma = 72.19(1)-degrees, V = 620.6(2) angstrom 3 and D(calc) = 1.34 g cm-3 for Z = 1. Least-squares refinement based on 1794 observed reflections (I > 3-sigma(I)) converged at R = 0.059, R(w) = 0.080. I resides about a crystallographic center of symmetry and contains a planar Ga2N2 four-membered ring. The Ga2N2 ring has a mean Ga-N bond distance of 2.030(9) angstrom. The mean Ga-C bond distance in the dimethylgallium unit is 1.974(9) angstrom. The crystalline product [(i-Bu)Al-iminodibenzyl]2 (III), isolated from reaction of diisobutylaluminum hydride with iminodibenzyl, (C14H12)NH, in toluene, crystallizes in the triclinic space group P1BAR with unit cell parameters a = 10.767(2), b = 12.264(3), c = 13.230(4) angstrom, alpha = 75.57(2), beta = 74.14(2), gamma = 73.58(2)degrees, V = 1583.7(7) angstrom 3 and D(calc) = 1.16 g cm-3 for Z = 2. Least-squares refinement based on 2216 observed reflections (I > 3-sigma(I)) converged at R = 0.093, R(w) = 0.118. Compound III results from a unique condensation reaction in which ortho-metallation of one of the aromatic rings of iminodibenzyl was observed. Compound III has a mean Al-N bond distance of 2.036(7) angstrom. The mean Al-C(isobutyl) bond distance of 1.98(3) angstrom is comparable to 1.954(8) angstrom for the Al-C(aromatic) fragment.