N, S co-doped MnFe2O4@C magnetic nanoparticles were successfully synthesized by a simple method involving the preparation of MnFe2O4 nanoparticles and subsequent pyrolysis treatment. The physical and chemical properties of MnFe2O4, MnFe2O4@C and MnFe2O4@C-NS nanoparticles were characterized by X-ray diffraction (XRD), vibrating sample magnetometry (VSM), transmission electron microscopy (TEM), N2 adsorption-desorption and the pH at the point of zero charge. Their performances in the adsorption of Hg(II) from water were investigated. The adsorption process followed pseudo-second-order kinetics and the experimental data of equilibrium isotherms fitted well with the Langmuir model. MnFe2O4@C-NS showed the highest adsorption capacity of 108.56 mg/g, increasing more than 1.7 times compared to MnFe2O4. The enhanced adsorption performance was attributed to the larger specific surface area as well as the complexation of N and S ligands on the surface. The thermodynamic parameters of ΔH°, ΔS° and ΔG° at 30 °C were -24.39 kJ/mol, -0.046 kJ/mol K and -10.45 kJ/mol, respectively, which indicated that the adsorption of Hg(II) on MnFe2O4@C-NS was exothermic and spontaneous in nature. Moreover, MnFe2O4@C-NS showed superior selectivity towards Hg(II) compared with other metal ions generally present in mercury-containing industrial wastewater.