This study revealed the synthesis of cross-linked chitosan/Citrus reticulata peel waste (C/CRPW) composites that could be used as low-cost and green bio-adsorbents for the removal of Congo red (CR) dye from aqueous solutions. C/CRPW composites containing different amounts of Citrus reticulata peel waste (CRPW) and chitosan were prepared and cross-linked with glutaraldehyde. The composites were characterized by FESEM, FTIR, and BET. The C/CRPW composites as a new type of bio-adsorbents displayed superior adsorption capability toward anionic CR molecules and the adsorption capacities increased by incorporation of CRPW. Effects of different ambient conditions such as contact time, pH, adsorbent dosage, initial adsorbate concentration, and temperature were fully studied. The conditions which obtained 43.57 mg/g of the highest adsorption capacity were conducted at pH 4, initial concentration of 100 mg/L, adsorbent dosage of 2.0 g/L, and contact time of 24 hours at 328 K. The adsorption data was found to follow the pseudo-second-order kinetic model and the Freundlich isotherm model. According to the findings of this investigation, it was observed that the C/CRWP composites can be used as adsorbents due to their advantages of simple preparation process, environmentally friendly, renewable, efficient, and low-cost.