In this study, we proposed the solution plasma- (SP-) assisted green synthesis method using plants extracts, i.e., glucose, with the expectation of acting as a reducing agent and promotor for the formation of powder state of nanostructured MnO2. MnO2 was simply and rapidly synthesized within 10 min by the SP-assisted method. The structural features and morphology of as-synthesized MnO2 were characterized by XRD, Raman, FE-SEM, and TEM analyses. For potential application of as-synthesized MnO2, cationic dye, i.e., methylene blue (MB), removal performance was investigated by batch experiment at an initial concentration of C0 = 100 mg L−1. The obtained MnO2 exhibited effective dye removal ability given high C0, and simultaneously applied plasma discharging further enhanced removal efficiency. These contributions therefore open a new window not only on a powerful and environmentally benign synthesis route for efficient adsorbents but also on supporting multiple removal mechanism.