A new method of phase-modulated excimer laser crystallization to fabricate the three-dimensional nc-Si array within the a-Si∶H/a-SiN x∶H multilayers (MLs) is adopted. The results of atomic force microscopy (AFM), micro-Raman measurements and cross-section transmission electron microscopy (X-TEM) demonstrated that the crystallized sample shows a three-dimensional ordered structure of nc-Si with the average size of about 3.6 nm, which has longitudinal order with 14 nm periodicity confined by SiN x sublayers in the MLs, and lateral order with 2 μm periodicity by patterned local crystallization.