Enhancing the pseudocapacitive efficiency of layered double hydroxide (LDH) catalytic materials is vital for achieving higher energy densities in advanced electrochemical energy storage devices. In this study, we explore the impact of decorating NiCo LDH nanoflowers with NiS, ZnS, and NiZnS nanoflowers on their electrochemical behavior. The incorporation of ZnS and NiZnS markedly increases the porosity of the hierarchical nanoflower architecture relative to NiS, resulting in distinct surface-bonding features and improved interfacial charge transfer through synergistic interactions. Among the tested materials, hybrid NiZnS@NiCo LDH nanoflowers exhibit the highest performance, achieving C_sp of 2778 F/g at 1 A/g and retaining 86% of their capacity at 10 A/g after 3,000 cycles. Furthermore, an asymmetric supercapacitor assembled with NiZnS@NiCo LDH and activated carbon exhibits an energy density of 14.4 Wh/kg at a power density of 174 W/kg, maintaining 82% stability after 10,000 cycles. These findings underscore the morphological and interfacial advantages of NiZnS@NiCo LDH nanoflowers, with their exceptional cycling stability establishing them as reliable and efficient candidates for durable supercapacitors.