In this study, a fast and simple dissolution and coagulation method was adopted to produce polyethylenimine (PEI)-incorporated chitosan beads. The beads were characterized using FESEM, BET, TGA, and FTIR analysis. Evaluation of adsorption isotherms, adsorption kinetics, and thermodynamics support that the beads exhibit chemisorption, which process is spontaneous at low temperatures. The presence of 30% PEI content enhanced the adsorption capacity of chitosan beads by about two-fold, achieving a maximum of 183.15 mg/g as calculated from the Langmuir adsorption isotherm. Finally, the PEI-incorporated beads exhibited good regeneration and can maintain 94% performance across up to eight cycles which is a promising reusable dyes absorbent material to tackle water pollution on our environment.