The crystallization of amorphous Si (a-Si) thin films was performed using atomic layer deposition (ALD) of nickel oxide. Nickel oxide layers were deposited using nickel aminoalkoxide as a precursor in Ni and water as a precursor in oxygen. The presence of nickel oxide caused significant crystallization to occur in a-Si at 575 degrees C under a reducing atmosphere. Even one single ALD layer of nickel oxide was high enough to crystallize the a-Si thin films. Self-limiting layer controllability in ALD is useful in providing a catalytic layer for formation of polycrystalline Si thin films for application to large-scale flat panel displays.