Manganese oxides exhibit an excellent microwave absorption performance that could increase the degradation efficiency of organic pollutants in contaminated water. Incorporation of various transition metals into manganese oxides could bring about changes in their crystal structure and improve their physicochemical performance. In this work, a better microwave absorption material was obtained by adjusting and controlling the electron spin magnetic moments of Fe-doped birnessite. The powder X-ray diffraction, inductive coupled plasma emission spectrometer, X-ray photoelectron spectroscopy, and network analyses were performed to characterize the crystal structure, chemical composition, valence and content of the elements, and the microwave absorption performance of the obtained samples. Doping Fe into birnessite resulted in little changes to their crystal structure. The narrow energy spectrum of Fe (2p) revealed that the doped Fe was in the form of Fe (III) in birnessite structure. As the content of Fe (III) increased, the content of Mn (III) decreased accordingly. Substitution of Mn (III) by Fe (III) in the birnessite crystal lattice, confirmed by combining the characterization analyses with structure refinements for each doped sample, increased the overall numbers of unpaired electrons in birnessite structure, resulting in a higher electron spin magnetic moment and better microwave response. Compared with the non-doped sample, Fe-doped birnessite improved the efficiency of tetracycline degradation, which proved that Fe-doped birnessite indeed had better response towards the microwave, and thus, could be utilized for better removal of organic pollutants under microwave irradiation. (C) 2017 Elsevier B.V. All rights reserved.