The development of electromagnetic wave (EMW) absorption materials with lightweight, wide absorption bandwidth, thin thickness, and strong EMW absorption performance has become a hotspot. Herein, the morphologycontrolled preparation of α-manganese dioxide (α-MnO 2 ) was successfully obtained via a facile hydrothermal method, and the EMW absorption performance of α-MnO 2 was investigated in detail. The results indicated the asobtained Mn-1.0-120 possessed the best EMW absorption performance with minimum reflection loss of −53.43 dB at about 5.2 GHz with a thickness of 4.1 mm originated from the synergistic effects of multiply scattering, dielectric loss, and magnetic loss. This contribution demonstrates that the MnO 2 has promising candidates with a tunable EMW absorption performance for applications in the electromagnetic field in the future.