It has been demonstrated that Raman spectroscopy is an excellent technique for the characterisation of the graphite in flake and spheroidal cast irons. The Raman spectrum of graphite is highly sensitive to both structural ordering and residual stresses as can be seen from the position, intensity and shape of the Raman bands. The relative intensities and widths of the G Raman bands for flake and spheroidal graphite have been compared and found to correspond to the degree of graphitisation across the graphite. The two Raman bands of the G doublet (G₁ and G₂) change in intensity and width with distance across a graphite spheroid, although their positions remain approximately constant. In contrast, the change in intensity and width of the two Raman bands of the G doublet for flake graphite shows no discernible pattern leading to the conclusion that there is no systematic change of graphitic ordering along a graphite flake. Finally, the fact that the positions of the G₁ and G₂ Raman bands for both flake and spheroidal graphite remain relatively constant with distance implies that there are no residual stresses in the graphite in flake and spheroidal cast iron.