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The anchoring of alumoxane, synthesized by the in situ hydrolysis of trimethylaluminum, on the internal pore walls of a mesoporous MCM-41 support generates a highly active and selective host for bis(cyclopentadienyl)zirconium dimethyl (Cp2Zr(CH3)2) in the oligomerization of propene. The regioselective preference of the immobilized metallocene is preserved and a typical Flory–Schulz distribution for the propene oligomers is obtained.