Heavy metals are considered a class of contaminant that can accumulate in the food chain and thus must be removed from contaminated media. Heavy metals can be removed by electrocoagulation, electroflotation, electrodialysis, capacitive deionization, and so on. Among the methods to remove heavy metals, capacitive deionization is one of the most attractive methods that can remove heavy metal ions without using a large volume of chemicals and producing a high number of heavy metals containing solid wastes. In this study, after a brief introduction to the mechanism of capacitive deionization, we focus on materials that have been developed as electrodes for heavy metal removal in capacitive deionization and summarize the latest advancements. Finally, with particular emphasis on material design, we provide some further insights in this area.