AbstractThe utilization of heterostructured electrodes offers an effective approach to boost the energy density of supercapacitors without sacrificing their power density. However, the adoption of such materials is frequently impeded by sluggish reaction kinetics. Herein, an island‐like CoNi2S4@NiCo‐layered double hydroxide/biomass carbon (CoNi2S4@NiCo‐LDH/BC) heterostructure is synthesized by embedding CoNi2S4 in the interlayer of NiCo‐LDH nanosheets on BC through a partial in situ sulfidation process. Theoretical and experimental analyses indicate that this unique structural configuration lowers transport barriers and enhances ion adsorption capacity, leading to a significant improvement in ion/electron reaction kinetics. In addition, the embedded structural design effectively alleviates the significant volume expansion during charge–discharge process, while the robust BC framework prevents electrode degradation, thereby enhancing stability. These advantages enable the developed electrode material to achieve a high specific capacity (1655.75 C g−1 at 1 A g−1) and an extended cycle life (86.82% capacity retention after 10 000 cycles). Significantly, the assembled hybrid supercapacitor CoNi2S4@NiCo‐LDH/BC// activated carbon demonstrates a remarkable energy density of 95.57 Wh kg−1 at 866.61 W kg−1 and exceptional cycling stability, maintaining 95.16% capacity after 10 000 cycles. This research offers an effective strategy to promote ion/charge transfer and adsorption capacity of heterostructure and provides a new approach to the development of advanced supercapacitor electrodes.