Red mud, a Fe-rich waste generated from the aluminum industry, was recovered as an adsorbent for wastewater treatment. The separation process of red mud from water after adsorption, including centrifugation and filtration, was complicated. This study demonstrated an alternative option to recycle red mud for preparing magnetic adsorbent via a facile hydrothermal route using ascorbic acid as reductant. Red mud is weakly magnetized and consists of andradite, muscovite, hematite, and cancrinite. After hydrothermal treatment, andradite in red mud was reductively dissolved by ascorbic acid, and transformed into magnetite and morimotoite. With increasing hydrothermal temperature, the dissolution of andradite accelerated, and the crystallite size of magnetite increased. When the hydrothermal temperature reached 200 °C, the prepared adsorbent P-200 showed a desirable saturation magnetization of 4.1 Am2/kg, and could be easily magnetically separated from water after adsorption. The maximum adsorption capacity of P-200 for Zn2+ was 89.6 mg/g, which is eight-fold higher than that of the raw red mud. The adsorption of Zn2+ by P-200 fitted the Langmuir model, where cation exchange was the main adsorption mechanism. The average distribution coefficient of Zn2+ at low ppm level was 16.81 L/g for P-200, higher than those of the red mud (0.3 L/g) and the prepared P-120 (1.48 L/g) and P-270 (5.48 L/g), demonstrating that P-200 had the best adsorption capacity for Zn2+ and can be served as a practical adsorbent for real-world applications. To our knowledge, this is the first study to report the conversion of red mud into a magnetic adsorbent under mild conditions.