Capacitive deionization (CDI) is a promising electrochemical water treatment technology. Development of new electrode materials with higher performance is key to improve the desalination efficiency of CDI. Carbon nanomaterials derived from metal–organic frameworks (MOFs) have attracted wide attention for their porous nanostructures and large specific surface areas. The desalination capacity and cycling stability of MOF-derived carbons (MOFCs) have been greatly improved by means of morphology control, heteroatom doping, Faradaic material modification, etc. Despite progress has been made to improve their CDI performance, quite a lot of MOFCs are too costly to be applied in a large scale. It remains crucial to develop MOFCs with both high desalination efficiency and low cost. In this review, we summarized three modification methods of MOFCs, namely morphology control, heteroatom doping, and Faradaic material doping, and put forward some constructive advice on how to enhance the desalination performance of MOFCs effectively at a low cost. We hope that more efforts could be devoted to the industrialization of MOFCs for CDI.