The treatment of pyrrolidine(C_4H_8NH) with sequentially trimethylaluminum and carbodiimide Cy N=C=NCy in a molar ratio of 1:1:1 in the presence of O_2 afforded a new guanidinatoaluminum complex, [{(C_4H_8N)C(NCy)_2}Al Me(μ-OMe)]2(1), which was characterized by elemental analyses, ~1H, ^(13)C NMR spectra and single-crystal X-ray diffraction analysis. Complex 1 crystallizes in monoclinic, space group P21/c with a = 9.8330(9), b = 8.5786(8), c = 24.159(2) ?, β = 92.927(2)°, V = 2035.3(3) ?3, Dc = 1.141 g cm-3, F(000) = 768 and μ = 0.110 mm-1. In addition, complex 1 was used to catalyze the Meerwein-Ponndorf-Verley(MPV) reduction and 1 as a pre-catalyst at low catalyst loadings(5 mol%) exhibited good catalytic activity for the reduction of a series of aldehydes to the corresponding alcohols in good yields(conv. up to 99%).