Super activated carbon is a promising electrode material for capacitive deionization (CDI), an emerging sustainable desalination technology. Increasing its CDI performance requires improving hydrophilicity while maintaining high specific surface area. Traditionally this is challenging, but modifying super activated carbon with earth-abundant metal ions at room temperature can achieve both aims through a low-energy process aligned with sustainability. The modified super activated carbon showed higher specific surface area, improved hydrophilicity, and enhanced desalination performance. Particularly, the salt adsorption capacity of Cu2+-modified super activated carbon in 500 mg/L NaCl solution at 1.2 V increased from 35.4 mg/g to 49.3 mg/g, among the highest for sustainable carbon materials. The capacity increase was enabled by simultaneously increasing specific surface area and hydrophilicity through themetal modification process. Along with high charge efficiency (93.4%), fast adsorption rate, and good cycling stability (80% capacity retention over 50 cycles), the modified super activated carbon displayed superior overall desalination performance. This study exemplifies how sustainable design principles can be applied to synthesize high-performance CDI electrode materials, through green chemistry and engineering for optimized efficiency.