The catalyst {[(2-ArN == C(Me)(2C5H3N]FeCl2} (Ar = 2-C6H4(i-Pr)) with methylaluminoxane (MAO) as cocatalyst was intercalated between layers of montmorillonite (MMT) for ethylene oligomerization. Metallocene catalyst Me2Si(Ind)2ZrCl2 and MAO was then added to form a dual functional catalytic system. A PE/MMT nanocomposite was prepared by copolymerization of ethylene with α-olefins produced in situ from ethylene over the dual functional catalytic system. The catalytic system was of high polymeric activity. The resultant PE/MMT nanocomposites were stable and got increases in tensile strength and temperature of maximum weight loss (Tonset).