Metachromatic properties of admixture of thionine and methylene blue(MB) in aqueous solution and phospholipid bilayer membrane have been studied by absorption spectroscopy. When thionine and MB were mixed, new coaggregate has been formed because of MB was redistributed to thionine aggregate. In phosphlipid bilayer membrane system, the highly concentrated thionine was easily formed the coaggregation with MB moiety independent of MB concentration, and absorption band of admixture were more transferred to short wavelength than aqueous system. In monomeric thionine concentration, the coaggregation band was observed at the middle wavelength between the site of monomeric thionine and the site of dimeric MB in the presence of lipid bilayer membrane.