Red mud, a solid waste produced in large quantities, possesses a high specific surface area and is rich in metal oxides, making it a promising material for adsorbent preparation. However, its practical application is constrained by its relatively low adsorption capacity and the potential environmental risks it poses. This study focused on the preparation of modified red mud (MRM) with enhanced adsorption performance for Ni2+ using a hydrothermal method involving sodium hydroxide and colloidal silica. The maximum adsorption capacity of MRM for Ni2+ reached 8.22 mmol·g–1, a substantial improvement compared to raw red mud (0.28 mmol·g–1) and sulfuric acid-activated red mud (0.46 mmol·g–1). The pseudo-second-order kinetic and Langmuir isotherm models accurately described the monolayer chemical adsorption process of Ni2+ on MRM. Additionally, leaching tests with simulated rainwater demonstrated that Ni-loaded MRM exhibited high stability, suggesting its potential for safe stockpiling or repurposing, such as in construction materials. Sequential extraction, XRD, FT-IR, and XPS results revealed that cation exchange was the primary mechanism in the adsorption process, with Ni2+ being immobilized within the zeolite framework structure of MRM, contributing to its strong adsorption stability. Inner-sphere complex formation also played a role in Ni2+ adsorption. In conclusion, this method offers an effective approach to both red mud utilization and heavy metal removal from wastewater, presenting a practical solution for waste management through resource recovery and environmental remediation.