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Graphite and various carbonaceous compounds are widely used in industry and nanotechnology as modern high-tech constructural materials. These comprise graphene layers forming bundles and crystallites, whose size and packing are of great importance for macroscopic properties. That is why non-destructive structural methods allowing determination of crystallite size and their ordering.are of major interest. Laser Raman micro-spectroscopy which uses modern laser Raman spectrometers of last generation, such as T64000, LabRAM HR Horiba-Jobin Yvon equipped by high-sensitive CCD detectors and microscopes, allow one to identify various carbon modifications, because each of the latter exhibits its own specific Raman spectrum, characterized by a given number of Raman lines with their particular parameters (frequency, intensity, half-width, contour). Besides, this non-destructive method gives a unique possibility of Raman micro-mapping of the samples, that is, obtaining information about sample heterogeneity. In this study the method was applied to many samples of various types. These are carbonaceous materials of natural origin (graphites of various genesis, shungites, meteorites, living matter ), as well as industrial origin, such as glassy carbon, diamond-like carbon, nanotubes, fibers, graphen, etc).