Metal-Induced Crystallization (MIC) of amorphous silicon (a-Si) using aluminum and nickel as catalysts were performed with a variation of metal thickness and temperature. Raman results showed that the crystallization of a-Si depended on the thickness of aluminum while not on nickel. Nickel that forms silicide nodules during annealing simply catalyzed the formation of crystalline silicon (c-Si) while aluminum was consumed and transferred during MIC, which resulted in more complex microstructural characteristics. Crystalline silicons after NIC had elongated shape with a twin along the long axis. Morphological change after Aluminum-Induced Crystallization (AIC) showed more equiaxial grains. The nucleation and growth mechanism of AIC was discussed.