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This research confirmed the chemical structure of Curcumine and Carthamin pigments whose pigments were separated and refined from the Curcuma longa and Carthamus Tinctorious which were natural dye using FT-IR, HPLC and so on. The cotton and the silk fabrics were dyed using a main pigment and then this research obtained the conclusion as it follows. The curcumine, the main pigment of Curcuma longa extracted from the mixed solvent of acetic anhydride and methanol (CH3OH), had the maximum absorption wavelength at 504.0 nm and was confirmed as yellow natural pigment. The Carthamin, the main pigment of Carthamus Tinctorious extracted from the mixed solvent of dichloromethane and methanol, had the maximum absorption wavelength at 420.0nm. This pigment was confirmed as yellow natural pigment. The dyeing property of the main pigment about the silk fabrics was superior to that about the cotton in both the Curcuma longa and Carthamus Tinctorious, and the dyeing property of Carthamus Tinctorious was superior to that of Curcuma longa.