Aluminosilicate solid waste, primarily comprising red mud, coal gangue, fly ash, and tailings, is characterized by high annual production, low comprehensive utilization rate, and significant environmental damage. Currently, there is an urgent need for effective methods to manage and valorize aluminosilicate solid wastes. Thermodynamic investigations enable the assessment of phase transition behaviors, process conditions (such as temperature and pressure), and the direction and feasibility of reactions. Moreover, thermodynamics can predict the composition of resulting products and reveal the reaction mechanisms. All the aforementioned issues are instrumental in refining solid waste treatment processes and achieving efficient use of resources. Therefore, to promote the application of aluminosilicate solid waste, this paper describes the predictive and guiding functions of thermodynamics in the utilization of solid waste, focusing on three aspects: composition design, ceramization, and process optimization. Additionally, current challenges and future trends are discussed herein.