In this paper, the dye sludge which was prepared from Congo red solution by flocculation method was further modified by catechol and 1, 6-hexanediamine before usage to remove Cr(VI) ions. This particles were characterized by multiple testing means and the effects of removal, such as contact time, pH value, initial concentration, and temperature, were studied by batch mode. The maximum adsorption capacity of Cr(VI) was 282.48 mg/g and the whole process was spontaneous and endothermic. Hopefully, with the advantages of facile preparation and high adsorption capacity, the dye-based adsorbent has broad application prospects in the field of wastewater treatment.