Biomass-derived raw bamboo charcoal (BC), NaOH-impregnated bamboo charcoal (BC-I), and magnetic bamboo charcoal (BC-IM) were fabricated and used as bio-adsorbents and Fenton-like catalysts for methylene blue removal. Compared to the raw biochar, a simple NaOH impregnation process significantly optimized the crystal structure, pore size distribution, and surface functional groups and increase the specific surface area from 1.4 to 63.0 m /g. Further magnetization of the BC-I sample not only enhanced the surface area to 84.7 m /g, but also improved the recycling convenience due to the superparamagnetism. The maximum adsorption capacity of BC, BC-I, and BC-IM for methylene blue at 328 K was 135.13, 220.26 and 497.51 mg/g, respectively. The pseudo-first-order rate constants at 308 K for BC, BC-I, and BC-IM catalytic degradation in the presence of H O were 0.198, 0.351, and 1.542 h , respectively. A synergistic mechanism between adsorption and radical processes was proposed.