AbstractN-M ethyl-2-dimethylaluminium pyrrolide, (CH3)2Al -C4H3NCH3, crystallizes in the triclinic space group P1̄ with the lattice constants a = 700.5(1), b = 725.9(1), c = 886.8(1) pm, α = 67.69(1)°, β = 70.99(1)°, γ = 88.48(1)°, and Z = 2. This compound is isotypic with the gallium homologue [1], the shortest metal-ring contact between the two molecules of one unit cell decreases to 228.6 pm. N-dimethylgallium tetramethylpyrrolide has been synthesized from Li-N (CCH3)4 and (CH3)2GaCl. This “π-associate” crystallizes in the monoclinic space group P21/c with the lattice parameters a = 989.9(2), b = 1305.4(3), c = 878.3(2) pm, β - 112.73(1)° and 4 units per cell. Again two centrosymmetrically orientated molecules form a dimer by short (224.0 pm) intermolecular “Ga - πC ” contacts but the structure differs significant from the structure of the indium homologue [1].