The steepest descent method, one of the least square method was applied for the estimation method for thecarbon layer size distribution proposed by Diamond and the reliability was examined with X-ray diffraction patternsof mesocarbon microbeads heat-treated at lower temperatures. The layer size distribution calculated by the conventional matrix method showed negative histograms, whereas the method applied in the present study showed no such histogramswhich made possible to discuss about the relation between the heat treatment temperature and the average size anddistribution of carbon layer.