In the present research, a biopolymer Chitosan (C) grafted with ethylenediamine (EDA) and methyl acrylate (MA) were compared for the adsorption of Congo red dye from aqueous phase. The grafted chitosan product was characterized by Fourier transform infrared spectroscopy (FTIR), Scanning electron microscopy (SEM), Differential scanning calorimetry (DSC), X-ray diffraction (XRD) and point of zero charge to study the change in mechanical and thermal properties. The effects of process variables like adsorbent loading, initial dye concentration, initial solution pH, contact time and temperature on adsorption phenomena were investigated. The equilibrium isotherm data was analyzed using Langmuir and Freundlich isotherm models, and the adsorption followed the Langmuir isotherm model (R = 0.992 and 0.991 for EDAC and MAC, respectively). The maximum adsorption capacity of EDAC and MAC for Congo red uptake calculated from Langmuir isotherm model was 1607 mg/g and 1143 mg/g, respectively. The adsorption kinetics was studied using pseudo 1st and 2nd order models. Pseudo second order rate model provided the best fit for both grafted adsorbents with R ≥0.99. The values of Gibbs free energy (-9.628 and -8.878 kJ/mol), enthalpy (44.9 and 42.2 kJ/mol) and entropy (0.18 and 0.17 J/mol·K) revealed spontaneous and endothermic adsorption of Congo red onto EDAC and MAC surface. The pollutant adsorption test indicated that chitosan grafting with ethylenediamine is superior to Methyl acrylate grafting agent.