Novel chitosan-modified magnetic graphitized multi-walled carbon nanotubes (CS-m-GMCNTs) were synthesized via a suspension cross-linking method. Composition, morphology and magnetic properties of as-prepared CS-m-GMCNTs were characterized by XRD, SEM-EDS, BET and VSM. The large saturation magnetization (12.27 emu g(-1)) allows fast separation of CS-m-GMCNTs from treated aqueous solution. The adsorption of congo red (CR) on CS-m-GMCNTs was strongly dependent on pH, temperature of the aqueous phase and adsorbent dosage. Up to 100 and 94.58% color removal could be achieved in 100 min contact time with 10 and 50 mg L-1 of initial concentrations, respectively. The adsorption capacity of CR onto CS-m-GMCNTs could reach 262.9 mg g-1. The pseudo-second-order kinetic model with high correlation coefficients (R-2 >0.999) was suitable to describe the process of CR adsorption onto CS-m-GMCNTs. The Langmuir model fitted the adsorption isotherm data better than the Freundlich model. Values of thermodynamic parameters (4G, 4H and A,S) indicated that the adsorption process was strongly dependent on temperature of the aqueous phase, and spontaneous and endothermic process in nature. Therefore, CS-m-GMCNTs adsorbent displays main advantages of excellent dispersion, convenience separation and high adsorption capacity, which implies their potential application in the environmental cleanup. (C) 2013 Elsevier B.V. All rights reserved.