This study investigates the properties of H2-reduced calcium-added bauxite residue, self-hardened pellets, and the feasibility of iron recovery through electrostatic and magnetic separation methods. The oxide pellets are prepared via a mixing of bauxite residue, calcite, and quicklime. The self-hardened pellets are reduced at 1000 °C with hydrogen gas flow for 120 min. The chemical composition, phase identification, and microstructural observations are executed using X-ray fluorescence (XRF), X-ray diffraction (XRD), and scanning electron microscopy (SEM), respectively. The porosity and strength of the self-hardened pellets are performed by the Mercury intrusion porosimetry and tumbling tests, respectively. The separation of iron is examined through a dry electrostatic technique, and in wet conditions, i.e., via Davis Tube and low-intensity magnetic separation (WLIMS). The effect of the magnetic field (0.1, 0.25, and 0.32 T) is tested on two different particle size fractions (−212 + 106 µm and −106 + 74 µm). It is found that most of the iron oxide in the bauxite residue is converted to metallic iron, which corresponds well with both XRD and SEM results. The Carpco electrostatic tests indicate that this approach is inefficient for the studied type of material because of the intensive association of iron with the rest of the components leading to transferring it to the middling rather than to conductive product. However, both the Davis Tube and WLIMS approve a reasonable improvement in the Fe content from 22% to 37% with acceptable recoveries. The results of the Davis Tube show that there is an optimum magnetic field and particle size for maximization of Fe grade and recovery. Finally, further suggestions are highlighted for the physical beneficiation of studied bauxite residue with the purpose of maximizing iron grade and recovery.