We recount the study of plates cut from natural diamonds of mineralogical types I and IV with the use of optical polarization microscopy, photo-and cathodoluminescence (CL). A series of specimens exhibited two macroscopic zones of different structures characterized by the alternation of crystalline regions with different nitrogen contents. Diamonds are block structures with a lower nitrogen content. CL spectra were observed from central, intermediate, and peripheral zones of the plates. The crystal growth mechanism is discussed, and an attempt is made to correlate the spectroscopic measurements with the CL images formed in a color SEM. The findings may be useful in establishing a criterion to assess diamonds for certification.