The half-titanocene (eta(5)-pentamethylcyclopentadienyl)tribenzyl titanium (Cp*TiBz(3)) with methylaluminoxane (MAO) as the cocatalyst was employed to catalyze propene polymerization at ambient pressure. A novel atactic polypropene elastomer with a high molecular weight ( (M) over bar(w) = 2 - 8 x 10(5)) was produced. The effects of the polymerization conditions on the catalytic activity and polymer molecular weight are discussed. C-13 NMR analysis confirmed that the catalyst system Cp*TiBz(3)/MAO produced atactic polypropenes, and the polymerization mechanism was in agreement with the Bernoullian process. The triad sequence distribution of the polymer was measured and found to be as follows: mm = 6.15%, mr = 40.87%, and rr = 52.98% (Bernoullian factor B = 1.03); this indicated that the insertion of propene with the catalyst system followed a chain-end control model.