Thallium (T1), is a highly toxic trace metal in the natural environment. Emerging TI pollution in waters has gradually become a global concern. However, limited removal technologies are available for Tl-containing wastewater. Herein, MnFe2O4-biochar composite (MFBC) was successfully fabricated via coprecipitation method as a novel and efficient adsorbent for treating Tl(I)-contaminated wastewater. It was found that the MFBC, with a specific surface area of 187.03 m(2)/g, exhibited high performance across a wide pH range of 4-11, with the superior Tl(I) removal capacity (170.55 mg/g) based on Langmuir model (pH 6.0, a dosage of 1 g/L). The removal mechanisms included physical and chemical adsorption, ion exchange, surface complexation, and oxidation. This investigation revealed that MFBC is a promising and environmentally friendly adsorbent with a low cost, large specific surface area, magnetic properties, and high efficiency for the removal of Tl(I) from wastewater.