This paper describes a study of the nucleation and growth of graphite crystal of levitation melted high purity Fe-C-Si alloys with emphasis on hypereutectic composition. Spherulitic graphite was observed to form at high purity alloy and converted to compacted by changing the starting iron from ultra-pure zone refined iron to 99.95 pct electrolitic iron. Residual C-C clusters might be acting as an effective nucleation site for graphite, and sulphur was the element to prevent graphite from nucleating. The graphite morphology changed from compacted to spherulitic as the sulphur content decreased.