Metal‐Organic Frameworks (MOFs), one type of porous materials with designable and tunable structures, are being actively studied as electrode materials in the supercapacitors (SCs) field. During the recent decade, various MOFs branches with special shapes and topological architectures have been studied. Among them, the pillar‐layered MOFs, the particular two‐dimensional (2D) frameworks, have gained much attention in energy‐storage fields. From the perspective of spatial topology, pillar‐layered MOFs can be divided into interpenetrating and non‐interpenetrating MOFs. These two MOFs with remarkable structures play different positive roles in SCs. In this review, we will focus on summarizing the current development of pillar‐layered MOFs from the two aspects: interpenetration and non‐interpenetration. Moreover, the strategies to improve the electrochemical performance of pillar‐layered MOFs as electrode materials are also discussed. We hope that this review could provide researchers with some new guidelines to develop high‐performance, energy‐saving and environmentally‐friendly MOF‐based materials for SCs in the future.
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