Metal-organic frameworks (MOFs), featuring tunable conductivity, tailored pore/structure and high surface area, have emerged as promising electrode nanomaterials for ion storage in capacitive deionization (CDI) and garnered tremendous attention in recent years. Despite the many advantages, the perspective from which MOFs should be designed and prepared for use as CDI electrode materials still faces various challenges that hinder their practical application. This summary proposes design principles for the pore size, pore environment, structure and dimensions of MOFs to precisely tailor the surface area, selectivity, conductivity, and Faradaic activity of electrode materials based on the ion storage mechanism in the CDI process. The account provides a new perspective to deepen the understanding of the fundamental issues of MOFs electrode materials to further meet the practical applications of CDI.