<p>Supercapacitors, particularly hybrid supercapacitors, have been a challenging area of research in recent years. The advantage of hybrid supercapacitors (HSCs) lies in their ability to metal–organic framework bridge the gap between the required energy density and the reported energy densities of electrical double-layer capacitors (EDLCs) and pseudocapacitors (PSCs). Generally, a HSC combines EDLC and PSCs -type electrodes in an asymmetric configuration. This asymmetric combination holds significant potential for utilization in various power-dependent devices. However, the energy-efficient application of HSCs demands innovation in several critical aspects. In this review, we address the recent developments in HSCs and their storage mechanisms. We focus on the engineering and innovations in electrode–electrolyte design, with special attention to aluminum-based metal–organic frameworks and their derived materials as electrodes. Furthermore, we illustrate electrochemical profile assessments, device fabrication strategies, and emerging applications. Finally, we elaborate on the existing challenges and future perspectives of HSCs.</p>