AbstractSince benzothiophene (BT) is a typical S‐containing compound in commercial fuels, proper adsorbents with desirable BT capture ability need to be developed. A novel magnetism‐bimetallic Fe3O4@Zn/Cu‐BTC composite has been synthesized via a simple one‐pot method for the removal of BT from mixed model fuel. SEM, XRD, XPS, and BET characterizations described the as‐prepared Fe3O4@Zn/Cu‐BTC. BT uptakes over Fe3O4@Zn/Cu‐BTC reached 85 mg/g, which is superior to those of previously reported in literature. Batch adsorption studies revealed that the adsorption process obeyed pseudo‐second order kinetic model, the determining step might be chemical sorption, and adsorption equilibrium could be achieved within 30 min. Among various isotherm models, the experimental data for adsorption of BT followed the Langmuir isotherm best. Thermodynamic parameters demonstrated that BT adsorption process was endothermic and spontaneous. Importantly, Fe3O4@Zn/Cu‐BTC could be easy obtained from liquid through Fe3O4 magnetism, and has high stability and good reusability, which might be beneficial for further practical deep desulfurization.