<p>Possessing high alkalinity, bauxite residue (red mud), a solid waste generated by the alumina refinery, is difficult to reuse. Adopting a simultaneous process to extract valuable metals along with lowering the alkali content in red mud is crucial for safe storage, effective reuse, and ecological sustainability. A sustainable acid-free hydrometallurgical process was proposed, which involves mechanical activation, alkali pre-treatment, and water leaching. The process parameters, like milling time, roasting temperature, leaching time, and temperature, were optimized to achieve maximum efficiency in recovery. Red mud activation and effective surface area enhancement were achieved with 30&#xa0;min of grinding, resulting in the successful recovery of approximately 90% of alumina and over 95% removal of alkali. The extracted alumina was precipitated as aluminum trihydroxide in its less alkali-incorporated form of bayerite. The final red mud residue with low alumina content can be used for the extraction of iron, TiO_2, and rare earth metals. Thus, this study highlights a practical way for the recovery and separation of alumina in a useful form from the waste red mud.</p> Graphical Abstract <p></p>