A new magnetic nanocomposite called MIL-100(Fe) @Fe3O4@AC was synthesized by the hydrothermal method as a stable adsorbent for the removal of Rhodamine B (RhB) dye from aqueous medium. In this work, in order to increase the carbon uptake capacity, magnetic carbon was first synthesized and then the Fe3O4 was used as the iron (III) supplier to synthesize MIL-100(Fe). The size of these nanocomposite is about 30–50 nm. Compared with activated charcoal (AC) and magnetic activated charcoal (Fe3O4@AC) nanoparticles, the surface area of MIL-100(Fe) @Fe3O4@AC were eminently increased while the magnetic property of this adsorbent was decreased. The surface area of AC, Fe3O4@AC, and MIL-100(Fe) @Fe3O4@AC was 121, 351, and 620 m2/g, respectively. The magnetic and thermal property, chemical structure, and morphology of the MIL-100(Fe) @Fe3O4@AC were considered by vibrating sample magnetometer (VSM), thermogravimetric analysis (TGA), zeta potential, X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), Brunner-Emmet-Teller (BET), and transmission electron microscopy (TEM) analyses. The relatively high adsorption capacity was obtained at about 769.23 mg/g compared to other adsorbents to eliminate RhB dye from the aqueous solution within 40 min. Studies of adsorption kinetics and isotherms showed that RhB adsorption conformed the Langmuir isotherm model and the pseudo second-order kinetic model. Thermodynamic amounts depicted that the RhB adsorption was spontaneous and exothermic process. In addition, the obtained nanocomposite exhibited good reusability after several cycles. All experimental results showed that MIL-100(Fe) @Fe3O4@AC could be a prospective sorbent for the treatment of dye wastewater.