A modified loess/chitosan composite (ML@CS) was prepared via solution. The microstructure and physicochemical properties of ML@CS were characterised via scanning electron microscope (SEM), Zeta potential, X-ray diffraction (XRD), Fourier transform infrared spectrum (FT-IR), and thermogravimetric analysis (TGA). An aqueous solution of methyl orange (MO) was used as simulated wastewater from which the influence of the initial concentration and pH of MO, the dosage amount and regeneration performance of ML@CS, adsorption temperature, and time on the adsorption effect of MO were systematically investigated. The adsorption kinetics, isothermal adsorption, and adsorption mechanism were also analysed. The results indicate that ML@CS had a good adsorption effect on MO. When the initial concentration of MO was 200 mg/L, pH was 5.0, and ML@CS dosage was 1.0 g/L, the adsorption equilibrium could be reached within 180 min at room temperature, and the equilibrium adsorption capacity and removal rate reached 199.52 mg/g and 99.75%, respectively. After five adsorption–desorption cycles, the MO removal rate remained above 82%. The adsorption behaviour of ML@CS for MO conforms to the pseudo–second–order kinetic model and the Langmuir isotherm adsorption model. The spontaneous exothermic process was mainly controlled by monolayer chemical adsorption and the physical adsorption only played an auxiliary role. ML@CS efficiently adsorbed MO in water and can be used as a high-efficiency, low-cost adsorbent for printing and dyeing wastewater treatment.