The development of high-quality supercapacitors relies heavily on the exploitation of composite electrode materials with well-defined nanostructures such as NiCo 2 S 4 (NCS). In this study, a two-step solvent-thermal approach was used to create a NiCo 2 S 4 @CoAl-LDH (NCS@CA) core−shell heterostructure for a light-assisted supercapacitor, yielding a noteworthy advancement in the properties of electrode materials. The resulting flowershaped NCS@CA nanosheets exhibit great potential for enhancing solar energy utilization. Compared to a solution without light, NCS@CA showed a noticeable increase in specific capacitance when exposed to light. As a result, NCS@CA demonstrated a robust specific capacity of 2120 F g −1 (120.4 F cm −3 ) when it was operated at 1 A g −1 . Also, the electrode showed excellent cycle life; after 10 000 cycles of charge and discharge, 98.96% of the total capacity was still preserved. Light-assisted supercapacitors possessing extraordinary electrochemical properties have been designed with activated carbon (AC) and NCS@CA as the working electrodes. The configuration exhibited an impressive energy density (35.1 Wh kg −1 at 751.2 W kg −1 ), representing a 36.6% improvement over nonlight conditions. The apparatus also demonstrated exceptional cycling stability, with the specific capacitance holding onto 97.7% after 10 000 cycles. These findings confirm that NCS@CA is a strong contender for building emerging systems for the storage of energy.