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A method for the preparation of well‐defined crystallites of MgCl2‐supported Ziegler‐Natta catalysts on Si wafers has been developed. This has been achieved by the spin‐coating of a MgCl2 solution onto a flat Si wafer, followed by controlled crystal growth to give well‐defined MgCl2 · nEtOH crystallites. The growth of the crystallites on the flat silica facilitates their characterization using electron and scanning probe microscopy. The relative proportions of 120° and 90° edge angles indicate the preference for the formation of a particular crystallite face for the MgCl2. Polyethylene has been identified to be formed on the lateral faces of the crystallite.magnified image