Four mesitylaluminum derivatives, Mes&(4-picoline)(C,H&5 (11, E t M e s a T H F (21, Mesz-CM-THF (31, and [Mes~Al(p-Cl)lz (4) (Mes = 2,4,64rimethylphenyl), have been prepared and their structures determined by single crystal X-ray diffraction methods. Compound 1 crystallizes in the monoclinic space group C2/c (No. 15): a = 43.784(15) A, b = 8.901(1) A, c = 16.760(2) A, p = 104.02(2)", 2 = 8, R = 10, and R, = 9.9. Compound 2 crystallizes in the orthorhombic space group P212121 (No. 19): a = 12.057(9) A, b = 13.490(3) A, c = 14.037-(2) A, 2 = 4, R = 5.4, and R, = 3.9. The halide derivative 3 crystallizes in the primitive monoclinic space group P21h (No. 14): a = 17.18(1) A, b = 14.754(2) A, c = 17.316(2) A, , 8 = 92.74(3)", 2 = 8, R = 6.5, and R, = 2.4. The base-free compound 4 exists as a dimer and crystallizes in the space group P21h (No. 14): a = 12.288(2) A, b = 15.824 (3) A, c = 9.095(2) A, / 3 = 108.43(2)", 2 = 4, R = 5.4, and R, = 5.9. The distortion associated with 1, 2, and 3 relative to the parent monomeric molecule, M e s a , is discussed with respect to substitution of the mesityl group for the C1 and E t ligands.