Dissimilar cation-anionic association of dyes («cyanine+oxyxanthene», «cyanine+sulfonepthalein») has been regularly investigated in aqueous solutions. Experimental (by spectrophotometry) and theoretical (by semiempirical) methods were used. The basic regularities of association processes have been discussed. It is shown that the change in the stability of associates has a systematic character both in the series of singly charged and doubly charged anions.