Electricity and water form an intricate nexus, in that water is crucial for power generation, and electricity (or other primary forms of energy) is the key enabler for water purification and waste-water treatment. Nonetheless, both energy conversion and water purification result in substantial amounts of greenhouse gas (GHG) emissions. These negative interactions with potential “snowball” effect, can be decoupled via the deployment of renewable power generation, and carbon capture from fossil-fuelled technologies. However, such retrofits pose new challenges as wind and solar energy exhibit intermittent generation patterns. In addition, integrating thermal power plants with carbon capture and storage (CCS) imposes energy penalties and increases water requirements. In the present research, an optimization framework is developed which enables systematic decision-making for the retrofit of existing power and water infrastructure as well as investment in renewable and green technologies. A key aspect of the applied framework is the simultaneous optimization of design and operational decisions in the presence of uncertainties in the water demand, electricity demand, as well as wind and solar power availability. The proposed methodology is demonstrated for the case of the water-electricity nexus in China, and provides in-depth insights into regional characteristics of low carbon electricity generation, and their implications for water purification and wastewater treatment, demonstrating a roadmap towards sustainable energy and electricity.