As a common type of pollutants in industrial wastewater, cationic dyes have attracted great attentions. Using biodegradable N,N-di (carboxymethyl) glutamic acid (GLDA) as ligand and corn stalk (CS) as matrix, a novel and green biomass modified material GLDA-CS was successfully prepared. The multifunctional property of GLDA-CS for removing methylene blue (MB), malachite green (MG) and alkaline red 46 (R-46) from wastewater was evaluated. The dyes were removed by the electrostatic adsorption based on the cationic adsorption properties of GLDA-CS. The removal rates of MB, MG and R-46 can quickly reach 90.4%, 96.8% and 94.8% in short time. especially for MG and R-46 even only 20 min. The adsorption capacities of the dyes still remain more than 86.5% of the initial values after 5 cycles. In a heterogeneous system, the dyes were removed by Fenton-like degradation based on the metal chelating property of GLDA-CS. 100% degradation rates of the dyes can be achieved in 35 min under the acidic region. Even if at pH 7, degradation rates are 44.1%, 47.1% and 56.6% higher than those under the conventional homogeneous system, and the degradation rate remained at 83.7% after 5 cycles. Regardless of the adsorption or degradation, GLDA-CS shows strong anti-anion interference ability. The potential mechanisms of adsorption and degradation for the dyes by GLDA-CS were deduced by quantization calculation. It is concluded that the adsorption removal of the dyes by GLDA-CS follows MG > R-46 > MB, and mainly depends on the electrostatic interaction between -COOH in GLDA-CS and -N- in the dye molecules. Based on the degradation mechanism of Fenton-like reaction, the possible active sites of the dyes attacked by free radicals and their possible degradation intermediates were predicted by the calculations of Fukui function.