Treatment of indolyl-3-aldimines(3-~tBuN=CH)C_8H_5NH with AlMe_3 afforded the deprotonated indolyl aluminum complex cis-[(μ-η~1:η~1-3-~tBuN=CH)C_8H_5NAlMe_2]_2,and its crystal structure was determined by X-ray single-crystal diffraction.The crystal belongs to the orthorhombic system,space group P2_12_12 with a = 14.590(9),b = 15.860(2),c = 13.266(8) A,μ=0.118 mm~(-1),M_r = 512.64,V= 3069.5(3) A~3,Z = 4,D_c= 1.109 g/cm~3,F(000) = 1104,R= 0.0451 and wR = 0.0937 for 4978 observed reflections with I> 2σ(I).In addition,the title compound exhibited a high catalytic activity toward the addition of amines to carbodiimide to form guanidines. Treatment of indolyl-3-aldimines (3 ~ tBuN = CH) C_8H_5NH with AlMe_3 afforded the deprotonated indolyl aluminum complex cis - [(μ-η ~ 1: η ~ 1-3- ~ tBuN = CH) C_8H_5NAlMe_2] _2, and its crystal structure was determined by X-ray single-crystal diffraction. The crystal belongs to the orthorhombic system, space group P2_12_12 with a = 14.590 (9), b = 15.860 (2), c = 0.118 mm -1, M_r = 512.64, V = 3069.5 (3) A~3, Z = 4, D_c = 1.109 g / cm~3, F (000) = 1104, R = 0.0451 and wR = 0.0937 for 4978 observed reflections with I> 2σ (I) .In addition, the title compound exhibited a high catalytic activity toward the addition of amines to carbodiimide to form guanidines.