The printing and dyeing industry discharges a large amount of dye wastewater, which causes serious pollution to the environment. Therefore, the removal of dyes in water is very important to the sustainable development of human society. Methyl orange (MO) is a common dye, whose removal has important representative significance. Layer double hydroxide (LDH) is an anionic layered compound with a brucite structure. Its physical and chemical properties can be precisely controlled by adjusting the ratio and type of anion and cation. LDH is often used as an adsorbent, electrocatalyst, etc. In this work, MO adsorption was studied using methoxy-modified NiFe- Layer double hydroxide (NiFe-LDH). A facile co-precipitation method was used to prepare NiFe-LDH, and a solvothermal treatment was used to modify NiFe-LDH with methoxy. The obtained methoxy-modified LDH was characterized by XRD, TEM, TG-DTG, DIS, etc. The effects of different pH values, dosages and MO concentrations on the adsorption performance of the samples before and after methoxy modification were investigated. In addition, the adsorption kinetics of the samples were also studied. Finally, it was found that the LDH modified with methoxy presented significantly improved MO adsorption performance, with a qm of 442.47 mg/m g, much higher than the single LDH adsorbent performance that has been reported so far. The reason may be due to the enhanced anion exchange capacity with MO resulting from the enlarged interlayer spacing, and the enhanced van der Waals attraction to MO molecules by methyl oxygen replacement.