Abstract In this work, thiol-functionalized MnFe2O4-MCM-41 (MnFe2O4-MCM-41-SH) was applied to remove Sb(III) from wastewater. Superparamagnetic MnFe2O4 nanoparticles were incorporated onto the thiol-functionalized MCM-41, which not only solved the aggregation problem of MnFe2O4 nanoparticles and the difficulty in separation of MCM-41, but also improved adsorption efficiency for Sb(III). The removal of Sb(III) by MnFe2O4-MCM-41-SH was investigated through batch experiments. The research results showed excellent adsorption performance and re-usability of MnFe2O4-MCM-41-SH. According to the Langmuir isotherm model, the maximum adsorption capacity of Sb(III) by MnFe2O4-MCM-41-SH is 164.8 mg/g. The Sb(III) removal efficiency was around 89.1% in the fifth cycle by MnFe2O4-MCM-41-SH with desorption treatment. On the basis of X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy, the Sb(III) removal mechanism was discussed. The reaction mechanism between Sb(III) and MnFe2O4-MCM-41-SH was complex, involving surface adsorption, oxidation, and reduction. In view of magnetic property and the high removal efficiency of Sb(III), MnFe2O4-MCM-41-SH is a promising adsorbent for Sb(III).