The ongoing discharge of desalination reject brine and emission of carbon dioxide (CO2) into the environment pose a major threat to the ecosystem. In this context, the Solvay process presents a potential mitigation scheme for reducing reject brine salinity while simultaneously sequestering CO2. This work reports for the first time a systematic techno-economic assessment of the conventional (ammonia-based) and modified (calcium hydroxide-based and Potassium hydroxide-based) Solvay processes. The model evaluates the effect of reactor conversion, inlet CO2 weight%, inlet CO2 temperature, gas/liquid ratio, and brine flow rate on the CO2 and Sodium ions removal. In addition, the process cost associated with each parameter was analyzed, and the impact of implementing carbon tax on process profitability was investigated. Furthermore, the Solvay processes were evaluated using economic metrics including Net Present Value (NPV), economy of scale, and Levelized cost of water. The results suggest that the calcium hydroxide-based modified Solvay process outperforms other processes in terms of CO2 and Sodium ions removal. Moreover, for the studied parameters, the calcium hydroxide-based modified Solvay process demonstrated economic viability, yielding a decent annual profit. However, the conventional Solvay process requires a remarkable amount of expenses, yet after the implementation of 40 dollars per metric tons of CO2 as a carbon tax, the conventional Solvay reaches the break-even point. These findings underscore the importance of implementing environmentally friendly practices in the industry, as the modified Solvay process proves to be a promising solution for mitigating environmental threats and promoting sustainable operations.