Naturally occurring Mn-rich limonite mainly composed of goethite and manganese oxides was used to remove tetracycline (TC) from the aqueous solution. The physicochemical properties of limonite were illustrated by various characterization techniques such as XRD, FE-TEM, XPS and FT-IR. The effects of dosage, initial solution pH, temperature and coexisting anions on TC removal were investigated. The results showed that TC could be efficiently adsorbed by limonite with high specific surface area and mesoporous structure through electrostatic interaction and complexation. The co-existence of PO43- inhibited the adsorption of TC by limonite due to the competition with TC for active sites. In addition, manganese oxides exhibited oxidative properties to TC, and the singlet oxygen (1O2) generated during the redox reaction was responsible for TC degradation. Furthermore, the regenerated limonite displayed an efficient recycling performance after four cycles. This study revealed that the Mn-rich limonite was a promising adsorbent for TC removal from aqueous solutions and promoted the application of natural mineral material in the environmental field.