FeOCl-MoS2 was synthesized via calcination, which possessed excellent adsorption performance for methyl orange (MO). The characterization results showed that the FeOCl-MoS2 was formed between MoS2 and FeOCl phases, while a remarkable improvement in specific surface area and porosity was obtained in comparison with pure FeOCl and MoS2. The adsorption experiment results showed that the adsorption capacity of MO dye at 25 degrees C could reach 1615.11 mg/g. In addition, the pseudo-second-order kinetic model (R-2 > 0.99) has a good applicability to describe the adsorption of MO onto FeOCl-MoS2. Langmuir isotherm model (R-2 > 0.99) can describe the adsorption process well, proving that the adsorption is surface-controlled monolayer adsorption. Thermodynamic analyses showed the adsorption is an exothermic process and has spontaneity in nature. The adsorption of MO onto FeOCl-MoS2 is attributed to electrostatic interaction. In particular, the adsorption capacity could still reach 82.1% of the initial adsorption capacity by alkali washing after five cycles. Hence, this study reveals that FeOCl-MoS2 could be a high-efficient adsorbent for dyes removal from wastewaters.