The degree of calcination of a dolomitic and a calcitic marble from Thassos Island, was investigated, by combining both Raman spectroscopy (RS) and X-Ray diffraction (XRD) techniques. The samples were prepared in isometric 2 cm cubes and calcined at three different temperatures, 900, 1050 and 1200 0C for 2 hours in order to produce quick lime. RS was applied at the lime sample’s surface and inner (near core) part after gently crushing. XRD was applied on the bulk rock specimens in order to verify the transformation process during heating of the raw material. Quality control of the applied calcination procedure is provided through the hydration of quick lime. The rise in solution temperature suggests the chemical “reactivity” of the produced slaked lime. Raman and XRD results revealed the presence of unburned quantities of calcite and dolomite on samples that were calcined at 900 0C. Furthermore, temperatures of 1050 and 1200 0C have shown comparable mineralogical features signifying evenly the conversion of carbonate minerals to their oxide equivalents, proving the completion of the calcination process. Finally, reactivity tests showed that the highest reactivity value of the produced quicklime, for both marbles is observed at the temperature of 1050 0C.