Industrial wastewater containing dyes is a significant burden to the environment. Many physicochemical methods have been used to remove these compounds. An interesting solution is the use of sorbents of natural origin. This paper describes a method for obtaining sorbents in the form of composite granules formed from a 2% alginate solution with the addition of 2.81% solution of graphene oxide (GO). The possibility of using the obtained granules for removing cationic dyes (Methylene Blue, Rhodamine B, Toluidine Blue, Victoria Blue B) and anionic dyes (Orange II, Congo Red, Methyl Blue) was investigated. As a result of the research it was demonstrated that the chemical and structural composition of the dye has a decisive influence on its sorption on composite granules. In cationic dyes, the number and order of amino groups are responsible for the rejection. In anionic dyes, on the other hand, the rejection factor increases with the number of sulfone groups. The granules obtained in the experiment can be successfully used to remove cationic dyes, achieving high rejection values (~100%), most quickly and efficiently removing dyes containing one such group (Toluidine Blue). In the case of anionic dyes, the highest rejection values (~80%) were obtained for Methyl Blue, which has three sulfone groups.