Controllable modulation strategies between onedimensional (1D) and two-dimensional (2D) structures have been rarely reported for metal−organic frameworks (MOFs). Here, 1D, 1D/2D, and 2D Ni−MOFs can be facilely prepared by adjusting the ratio of Ni 2+ and the pyromellitic acid linker. A low-dimensional structure can shorten the transmission distance, while MOFs with a high Ni 2+ content can supply rich active sites for oxidation− reduction reactions. The 2D structure Ni-MOF with an optimized Ni 2+ /pyromellitic acid ratio presents a good performance of 1036 F g −1 at a current density of 1 A g −1 with a comparable rate performance of 62% at 20 A g −1 . The study may offer a facile design to control the structure of MOFs for employing in electrochemical energy storage.