The treatment of pyrrolidine (C4HsNI-I) with sequentially trimethylaluminum andcarbodiimide CyN--C=NCy in a molar ratio of 1 :1:1 in the presence of O2 afforded a newguanidinatoaluminurn complex, [{(C4HsN)C(NCy)2}AIMe(/I-OMe)]2 (1), which was characterizedby elemental analyses, 1H, 13C NMR spectra and single-crystal X-ray diffraction analysis. ComplexI crystallizes in monoclinic, space group P21/c with a = 9.8330(9), b = 8.5786(8), c = 24.159(2) A,β= 92.927(2)°, V= 2035.3(3) A3, Dc = 1.141 g cm^-3, F(000) = 768 and μ= 0.110 mm^-l. In addition,complex 1 was used to catalyze the Meerwein-Ponndorf-Verley (MPV) reduction and 1 as apre-catalyst at low catalyst loadings (5 tool%) exhibited good catalytic activity for the reduction ofa series of aldehydes to the corresponding alcohols in good yields (cony. up to 99%).