Water is one of the fundamental resources for the existence of humans and the environment. Throughout time, due to urbanization, expanding population, increased agricultural production, and intense industrialization, significant pollution with persistent contaminants has been noted, placing the water quality in danger. As a consequence, different procedures and various technologies have been tested and used in order to ensure that water sources are safe for use. The adsorption process is often considered for wastewater treatment due to its straightforward design, low investment cost, availability, avoidance of additional chemicals, lack of undesirable byproducts, and demonstrated significant efficacious potential for treating and eliminating organic contaminants. To accomplish its application, the need to develop innovative materials has become an essential goal. In this context, an overview of recent advances in hydrogels based on chitosan and nanocomposites and their application for the depollution of wastewater contaminated with dyes is reported herein. The present review focuses on (i) the challenges raised by the synthesis process and characterization of the different hydrogels; (ii) the discussion of the impact of the main parameters affecting the adsorption process; (iii) the understanding of the adsorption isotherms, kinetics, and thermodynamic behavior; and (iv) the examination of the possibility of recycling and reusing the hydrogels.