We have fabricated multilayer assemblies consisting of cyanine dye and polyelectrolyte by means of alternate adsorption method. In this study we used two kinds of water soluble thiacyanine dyes and poly(diallyldimethylammonium chloride) (PDDA) as polycation. Anionic cyanine dye molecules were adsorbed onto the positively charged surface of PDDA layer, giving rise to the J-aggregate, The sequential alternate adsorption yielded the PDDA-(dye/PDDA)(n) assemblies (n, repeating number). UV-vis spectroscopy measurements indicated that peak absorbance at the J-band increased linearly with the increasing adsorption cycles. These results demonstrate the advantage of the alternate adsorption method for investigating J-aggregate-containing multilayer assemblies.