Recently a novel series of 2-substitutedimino-4-substitutedimino-6-(4- pyridineimino)amino-1,3,5-dithiazines (VIIIa1-a10) have been synthesized by refluxing 1-(4-pyridine)imino-5-substituted dithiobiuretes (Va-h) with various isocyanodichlorides (VIIa-c) in acetone-ethanol medium in 1:1 molar proportion for 2 hours. The structures of all the synthesized compounds were justified on the basis of chemical characteristics, elemental analysis and IR and NMR spectral analysis.