The experimental evaluation of structure formation in solutions of individual polymers, as well as in their mixtures with other polymers in order to predict the properties of materials obtained on their basis was the aim of this work. We used chitosan, sodium salt of chitosan succinyl, sodium salt of carboxymethyl cellulose, and polyvinyl alcohol. Distilled water, 1 % acetic acid, and buffer systems based on acetic acid and sodium acetate with pH = 3.80, 4.25, and 4.75 were used as solvents. It was found that the type of aggregates formed in polymer mixtures is determined by the nature of the solvent and the concentration of the polymers in the initial solution. A correlation has been shown between the nature of aggregates formed in solutions and some physicochemical properties of film materials obtained from solutions, namely, the degree of enzymatic hydrolysis, as well as the rate and degree of water vapor sorption by film materials. Thus, the studies carried out show that by varying the nature of the solvent, the concentration and nature of the polymers in the initial solutions, it is possible to control the structure formation in mixed polymer solutions, and, therefore, the properties of the resulting composites.