Due to their structural diversity, superior physiochemical characteristics, and promising electrochemical performance, metal-organic frameworks (MOFs) and layered double hydroxides (LDHs) have garnered substantial interest as potential materials for electrochemical energy storage and conversion. We provided three bimetallic layered double hydroxides (LDH): NiAl-LDH, CoAl-LDH, and ZnAl-LDH from aluminum-fumarate metal-organic frameworks (Al-Fum MOF) as a sacrificial template using a facile solvothermal method in an alkaline environment. Numerous materials containing aluminum are considered one of the best cathode materials for supercapacitors due to their applicability and structural tunability. These as-prepared active materials were sprayed on a nickel foam and used in three- and two-electrode setups. After conducting several electrochemical measurements such as CV and GCD, NiAl-LDH performed as the superior electrode with low charge-transfer resistance and higher capacity of 2.86 Ω and 373 F g−1, respectively. After assembling the asymmetric supercapacitor (ASC) system based on the NiAl-LDH, the maximum energy density of 8.65 Wh kg−1 at a power density of 155.58 W kg−1 was attained at the potential window of 1.5 V with the excellent cycling lifespan (∼ 95% retention) after 10,000 cycles. In this paper, we present a method for modifying a common material and developing it into new materials for future applications in energy storage.