Each year approximately 1.3 billion tons of food is either wasted or lost. One of the most wasted foods in the world is bread. The ability to reuse wasted food in another area of need, such as water scarcity, would provide a tremendous sustainable outcome. To address water scarcity, many areas of the world are now implementing desalination. One desalination technology that could benefit from food waste reuse is capacitive deionization (CDI). CDI has emerged as a powerful desalination technology that essentially only requires a pair of electrodes and a low-voltage power supply. Developing freestanding carbon electrodes from food waste could lower the overall cost of CDI systems and the environmental and economic impact from food waste. We created freestanding CDI electrodes from bread. The electrodes possessed a hierarchical pore structure that enabled both high salt adsorption capacity and one of the highest reported values for hydraulic permeability to date in a flow-through CDI system. We also developed a sustainable technique for electrode fabrication that does not require the use of common laboratory equipment and could be deployed in decentralized locations and developing countries with low-financial resources.