Layered double hydroxides (LDHs) represent a category of two-dimensional layered intercalation materials, showing significant potential as electrode materials for the production of high-energy-density supercapacitors due to their tunable composition, ease of synthetic modification, and low cost. Here, we constructed alkali-etched NiAl LDH-OH nanosheets/Ag nanoparticles (NPs) composite material (Ag@NiAl LDH-OH) for high-performance supercapacitors through a simple solvent-thermal reaction. The alkali treatment is employed to selectively etch some Al3+ ions, generating cation vacancies as active sites for energy storage. Additionally, under the simultaneous influence of strong alkalis and vacancies, the interlayer spacing of LDHs expands, aiding in the promotion of interlayer ion mobility. Meanwhile, the decoration of silver nanoparticles ensures excellent electron conductivity in the NiAl-LDH-OH nanosheets, thereby facilitating improved utilization of the active substance and achieving outstanding rate performance. The Ag@NiAl LDH-OH electrode, when prepared, demonstrates a significant increase in specific capacitance, reaching 1790 F g−1 at a current density of 1 A g−1. This represents approximately 7 times the specific capacitance of the pristine NiAl LDH electrode, with a capacity retention of 79 % even under a high current density of 20 A g−1. Moreover, the assembled asymmetric supercapacitor (ASC) attains a maximum energy density of 138.25 Wh kg−1 at a power density of 700 W kg−1, maintaining 81 % of its initial specific capacitance after 20000 cycles. This research introduces novel pathways for advancing high-energy-density SCs.