The dyeing effluent of high alkalinity, which could not be treated efficiently by traditional wastewater technologies, highlighted the need to explore a technically feasible, highly efficient and cost effective method. Thus, a fast and highly efficient method for the removal of dyes under alkaline conditions using magnetic chitosan-Fe(III) hydrogel was proposed. Firstly, chitosan-Fe(III) hydrogel was prepared by a chelation procedure with cheap and environmentally friendly chitosan and iron salts. We characterized the sorption and desorption of C. I. Acid Red 73, a common type of anionic dye, on magnetic chitosan-Fe(III) hydrogel, to understand its availability for alkaline dyeing wastewater. Sorption of dye to chitosan-Fe(III) hydrogel was fast (adsorption could reach equilibrium in less than 10 min) in a wide pH range, and agreed well to the Langmuir-Freundlich adsorption model with a high maximum adsorption capacity of 294.5 mg/g under pH = 12. Meanwhile, 1 mol/L NaOH was used to desorb the dye efficiently (desorption efficiency 94.4%) and 0.1 mol/L HCl was applied to regenerate the chitosan-Fe(III) hydrogel. The results showed that the chitosan-Fe(III) hydrogel could retain its high efficiency after the desorption and regeneration. The common coexisting ions almost had no negative effect on the dye adsorption of chitosan-Fe(III) and the removals of a variety of anionic dyes suggest that the magnetic chitosan-Fe(III) hydrogel could efficiently adsorb both the acid and reactive dyes under alkaline condition. Overall, the results reported herein indicated that magnetic chtisoan-Fe(III) with high adsorption efficiency and strong magnetic property is very attractive and implies a potential of practical application for alkaline dyeing effluent treatment.