Recently, metal–organic frameworks (MOFs), which are porous inorganic–organic hybrid materials consisting of metal ions (clusters or secondary building units) and organic ligands through coordination bonds, have attracted wide attention because of their high surface area, huge ordered porosity, uniform structural cavities, and excellent thermal/chemical stability. In this work, durian shell biomass carbon fiber and Fe₃O₄ functionalized metal–organic framework composite material (durian shell fiber-Fe₃O₄-MOF, DFM) was synthesized and employed for the adsorption removal of methylene blue (MB) from wastewater. The morphology, structure, and chemical elements of the DFM material were characterized by scanning electron microscope (SEM), X-ray diffraction (XRD), transmission electron microscope (TEM), and X-ray photoelectron spectroscope (XPS) techniques. Adsorption conditions such as pH, adsorption time, and temperature were optimized. The adsorption isotherm and kinetics results show that the adsorption process of DFM material to MB is more in line with the Freundlich model and pseudo-second-order kinetic model. Using these models, the maximum adsorption capacity of 53.31 mg/g was obtained by calculation. In addition, DFM material could be easily reused through an external magnet and the removal rate of MB was still 80% after five adsorption cycles. The obtained results show that DFM composite material, as an economical, environmentally friendly, recyclable new adsorbent, can simply and effectively remove MB from wastewater.