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Polymer-clay nanocomposites were fabricated from medium-density polyethylene and organically modified Na-montmorillonite (MMT) using the planetary ball milling as a new method. The materials were characterized using scanning electron microscopy, transmission electron microscopy, and X-ray diffraction (XRD). The crystalline size of polyethylene (PE) filled with MMT was studied using XRD. These studies indicated that the addition of MMT decreases the crystalline size of the polymer. Moreover, the degree of crystallinity of both ball-milled and un-milled PE and PE-clay nanocomposites was measured by applying the XRD technique. The results show that both milling time and clay content decrease the degree of crystallinity of PE.