The removal of dye contaminants from water is an important issue and different adsorbents have been developed for this purpose. Here, chitosan hydrogel, scaffold-chitosan hydrogel, and scaffold-chitosan hydrogel with activated carbon were developed and used in the adsorption of food blue 2 and food red 17, from single and binary aqueous systems. The adsorbents presented good mechanical properties, high efficiency, high adsorption capacity, and fast kinetics for single and binary systems. Chitosan hydrogel presented excellent reusability capacity and can be reused for five cycles. The use of these hydrogels enables the application of adsorbent materials with three-dimensional frameworks for dye adsorption in single or binary systems.