The reaction of organoaluminum derivatives, R3Al (R = Me, Et, Ph), with ((dimethylamino)methyl)ferrocene yields R3Al-N(Me2)CH2C5H4FeCp (R = Me (1a), Et (1b), Ph (1c); Cp = C5H5) quantitatively. The alkoxo and thiolato complexes, [Me2Al(mu-OC6F5)]2 and [Me2Al(mu-C10H7-2-S)]n, also react with ((dimethylamino)methyl)ferrocene to give Me2(C6F5O)Al.N(Me2)CH2C5H4FeCp (2) and Me2(C10H7-2-S)Al.N(Me2)CH2C5H4FeCp (3), respectively. Under similar reaction conditions ((dimethylamino)methyl)ferrocene does not react with tris(2,4,6-trimethylphenyl)aluminum (MeS3Al). The reaction of (2-C4H3S)3Al.OEt2 with the hydrated amine gives an aluminoxane [(2-C4H3S)2Al.N(Me2)CH2C5H4FeCP]2O (4). The resulting compounds have been characterized by H-1 and C-13 NMR spectroscopy. A single-crystal X-ray study of 1a established that it crystallizes in the monoclinic cell system, space group P2(1)/a (No. 14), with cell constants of a = 12.969(2) angstrom, b = 13.103(2) angstrom, c = 20.411(3) angstrom, beta = 91.45(2)-degrees, and Z = 8; R = 5.4% and R(w) = 3.7%, based on 2798 observed reflections (I(o) greater-than-or-equal-to 2.5sigma(I)). The molecular unit is monomeric with an Al-N bond distance of 2.06 angstrom. Compound 4 crystallizes in the monoclinic space group P2(1)/n (No. 14), with cell constants of a = 11.518(2) angstrom, b = 13.126(2) angstrom, c = 13.839(3) angstrom, beta = 96.14(1)-degrees, and Z = 2; R = 5.1% and R(w) = 5.0%, based on 2445 observed reflections (I(o) greater-than-or-equal-to 2.5sigma(I)). The molecular unit consists of two ferrocene moieties connected via an N-Al-O-Al-N linkage with Al-N and Al-O bond distances of 2.024 and 1.690 angstrom respectively. The NMR spectra of la and 4 are temperature dependent with significant changes occurring for the resonances associated with the Me2NCH2C5H4FeCp group.