Electrolyte systems are becoming increasingly important as the process industries transition to better address environmental sustainability and climate change. Industrial processes such as carbon capture and sequestration, brine water treatment, lithium refining, and many others require accurate and rigorous electrolyte thermodynamic models to support process simulation and design of chemical processes involving electrolyte systems. Distinctly different from nonelectrolyte systems, the solution nonideality of electrolyte systems is primarily characterized by the electrolyte solution chemistry and secondly impacted by the subsequent physical interactions and associations of true species in solutions. This Article presents the methodology in Aspen process simulators to address the solution chemistry with true species and apparent component approaches together with the two electrolyte thermodynamic models, Pitzer and Electrolyte Nonrandom Two-Liquid equations. Also covered are experimental data compilation, best practice in data regression, and industrial applications highlighted with CO 2 capture with amine solutions and high salinity brine solutions. We further present our perspectives in current challenges and emerging opportunities with thermodynamic modeling for electrolyte systems with high charge density ions, transport property estimation, and systematic data collection and verification.