The chitin thiocarbonate-Fe(II)-H2O2 redox system was investigated as the initiator for the graft copolymerization of acrylonitrile and acrylic acid monomers onto chitin powder. The reaction with vinyl monomers onto chitin was carried out under various parameters of the graft copolymerization reaction to elucidate the polymerization behavior in terms of graft yield. Reactions of chitin-acrylonitrile graft copolymer with hydroxyl amine hydrochloride, as well as, sodium hydroxide were conducted in order to obtain chitin-(amidoxime-co-acrylonitrile) and chitin-(acrylate-co-acrylamide) graft copolymers, respectively. The reaction efficiency depends upon the alkali concentration, time, temperature, and on the reactant concentrations. The prepared chitin derivatives were evaluated for use in the wastewater treatments for adsorption and desorption of heavy metal ions as well as acid and basic dyes.