A kind of NH₂-MIL-101(Fe)@viscose spunlaced nonwoven material (VSN) was prepared by in situ solvothermal method for the adsorption of organic dyes in wastewater and then carbonized in a tube furnace under N₂ atmosphere at 300 °C to improve the adsorption performances. The results showed that the synthesized NH₂-MIL-101(Fe) particles with a polyhedral structure were uniformly loaded on the VSN surface. After being carbonized, the NH₂-MIL-101(Fe)@viscose spunlaced nonwoven porous carbon material (VSNC) were obtained. Compared with uncarbonized NH₂-MIL-101(Fe)@VSN, the adsorption efficiency of NH₂-MIL-101(Fe)@VSNC for methylene blue (MB) significantly enhanced and could reach 98.3% under the condition of water bath temperature of 30 °C and pH 9. According to adsorption thermodynamic analysis, the MB adsorption process by NH₂-MIL-101(Fe)@VSNC was spontaneous. The quasi-secondary adsorption kinetic model was more suitable to describe the whole adsorption process of NH₂-MIL-101(Fe)@VSNC, implying that the adsorption mechanism of NH₂-MIL-101(Fe)@VSNC for MB was mainly chemical adsorption. NH₂-MIL-101(Fe)@VSNC presented good structure stability and reusability during the adsorption process. After being recycled five times, the MB adsorption efficiency still maintained about 86.3%.