The current peremptory for developing alternative resources to remunerate the ongoing energy burden worldwide has stimulated researchers to widen the horizon and push the boundaries toward creating sustainable and affordable solutions. Among the various existing energy storage devices, supercapacitorsSupercapacitors have gained extensive attention due to some of their intriguing properties. Albeit receiving constant regard, a fight for survival still exists when it originates to compete with the energy density of batteries. The pure electrostatic storage of charges which demands a high specific area and pseudocapacitors possessing poor electrical conductivityElectrical conductivity limits the wide application of supercapacitorsSupercapacitors in daily life. The aforementioned limitations for the introduction of advanced electrode materials to match the counterparts. Various 2D materials continue to revolutionize the field of energy storage because of their unique physiochemical properties like thin nanosheets and explicit surface area. Layered double hydroxidesLayered double hydroxides (LDHs) are lamellar materials that showcase superior ion tunability and better exposed active sites due to their layered structure. However, restacking the sheets is a possible limitation that can hamper the expected electrochemical performance. Therefore, it is inevitable to develop protocols to overcome this challenge. The incorporation of metal–organic frameworks (MOFs), a class of porous materials with high surface area can alleviate the layered double hydroxidesLayered double hydroxides (LDHs) materials for better performance. The resultant MOF/LDH heterostructure will combine the exclusive properties of both materials and provide synergistic benefits. This chapter extensively details the existing studies on MOFs and LDH materials, their properties, and their potential as next-generation energy storage devices, especially in the field of supercapacitorsSupercapacitors.