There is an urgent requirement to devise and develop highly-effective materials for the purification of industrial wastewater. Coloured effluents are particularly problematic due to their toxicity in plants, aquatic organisms and animals, dictating that polymeric adsorbents are highly sought for their capture.Chitosan hydrogels are a cost-effective substrate for the adsorption of dye molecules as they are contain a biopolymeric gelator that can form hydrogels with a polymer content as low as 3% by mass. Such materials are also highly suited for use within a biomedical context as carrier vehicles for the encapsulation and delivery of protein macromolecules, due to their hydrophilic nature. We disclose the capability chitosan-based hydrogels to non-covalently adsorb both reactive and disperse dye molecules, and a model anionic protein from aqueous solution. The materials generated offer both a platform for dye removal from industrial wastewater, and for the encapsulation and pH-mediated release of protein macromolecules.