Polypropylene was synthesized using binary metallocene catalysts, rac-ethylenebis-(1-η5-indenyl)-zirconium dichloride (rac-Et(Ind) 2 ZrCl 2 : Cata A) and zirconocene dichloride (Cp 2 ZrCl 2 : Cata B), in the presence of ZnEt 2 . The results indicated that ZnEt 2 was an effective agent in modulating isotactivity of polypropylene. Moreover, it was found that the [mmmm] pentad value of polypropylene prepared in the presence of diethyl zinc decreased to 84, and the new peaks of [rmmr] and [rmrr + mmrm] appeared, in contrast to the peaks from polyproplene obtained in the absence of diethyl zinc. Therefore, the possible reason was the occurrence of chain-shuttling polymerization in the CataA/CataB/ZnEt 2 catalyst system.