As porous coordination organic polymers, both metal–organic frameworks (MOFs) and their derived materials and MOF‐based composites offer unique organic or inorganic chemistries that display superior features of high specific surface area, accessible active sites, robust structural and chemical diversity, tailorable pore size, exceptional porosity, and pre‐ and postsynthesis structural tunability. Therefore, MOF‐based materials are attractive for energy storage applications, specifically for supercapacitor devices. This review presents recent progress in designing and utilizing pristine MOFs, MOF‐derived nanomaterials, and MOF‐based composite materials for supercapacitors. Most importantly, herein, recent highlights and classifications of electrolytes and their vital role in the structure–property correlation between the structures of MOF‐based materials and suitable electrolyte choices for ideal supercapacitor devices are discussed. Finally, together with a discussion of the progress and outcomes of MOF electrodes, the obstacles and prospects for future MOF‐related research and applications are discussed. To help this intriguing topic continue to advance, this review offers useful insights into the logical design of MOF‐based electrode materials.