The pulsed laser crystallization of amorphous silicon carbon (aSiC) thin films have been implemented by using XeCl excimer laser. The aSiC thin films were prepared on silicon and quartz substrates by pulsed laser deposition. The surface morphology, atomic order and phase of the asdeposited and post annealing films have been analyzed by atomic force microscopy (AFM) and Raman scattering spectroscopy. AFM results show that aSiC films can be nanocrystallized at a proper laser energy. The size of nanocrystals in the post annealing films increases with the laser energy density; the separation into crystalline silicon and carbon after laser annealing is identified through Raman analysis. The mechanism of the pulsed laser crystallization of aSiC films is discussed to account for the post annealing characteristics.