MnO6 octahedra without distortions in α-MnO2 have a low dipole content, which limits their dielectric loss capabilities. Herein, we develop protonated MnO2 with distorted MnO6 octahedra for increased dipole numbers via a two-step hydrothermal method. In comparison with α-MnO2, this protonated MnO2 provides greatly improved dipole polarization loss capabilities, resulting in a reflection loss value of -19.1 dB with an effective absorption bandwidth of 3.3 GHz at a low thickness of 2 mm.