The rapid growing demand for energy has necessitated the development of novel smart materials and structures in order to store the energy generated from renewables. Among various cross-functional platforms, metal–organic frameworks (MOFs) have emerged as an outstanding class of electrode materials for supercapacitor applications due to its porous structures and tunable functionalities. In this chapter, we elucidate the technical principles underlying the component design and nanostructuring that enhance the electrochemical properties of MOF-based electrode materials for supercapacitors. An in-depth examination of the fundamental engineering strategies for pristine MOFs, MOF composites, and their derivatives with various dimensionalities (0D, 1D, 2D, and 3D) for supercapacitors is explicated, elucidating the composition–structure–property correlations of the engineered MOF-based electrode materials. Finally, we discuss the challenges associated with MOF-based electrode materials for supercapacitors and possible solutions.