In the present study, nanoscale rod-shaped manganese oxide (MnO) mixtures were successfully prepared from graphitic carbon nitride (C3N4) and potassium permanganate (KMnO4) through a hydrothermal method. The as-prepared MnO nanomixtures exhibited high activity in the adsorption and degradation of methylene blue (MB). The as-synthesized products were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), surface area analysis, X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). Furthermore, the effects of the dose of MnO nanomixtures, pH of the solution, initial concentration of MB, and the temperature of MB removal in dye adsorption and degradation experiments was investigated. The degradation mechanism of MB upon treatment with MnO nanomixtures and H2O2 was studied and discussed. The results showed that a maximum adsorption capacity of 154 mg g−1 was obtained for a 60 mg L−1 MB solution at pH 9.0 and 25 °C, and the highest MB degradation ratio reached 99.8% under the following optimum conditions: 50 mL of MB solution (20 mg L−1) at room temperature and pH ≈ 8.0 with 7 mg of C, N-doped MnO and 0.5 mL of H2O2.