Nickel-cobalt hydrotalcite (NiCo-LDH) is widely acknowledged as a promising electrode material due to its high specific capacitance and energy density. However, in order to further enhance its cycle stability, the assistance of functional carbon materials is required. In this study, a superfine coal (FC) with an oxygen-enriched surface prepared through ball milling modification is incorporated into hydrothermal synthesis process of NiCo-LDH to form a composite known as NiCo-LDH/FC (NiCo-FC). When 0.325 g FC is added, the resulting NiCo-3FC exhibits an interlaced-structural characteristic along with excellent electrochemical properties and cycle stability. In a 6 M KOH electrolyte, NiCo-3FC demonstrates a significantly higher specific capacitance of 2101.03 F g−1 at a current density of 1 A g−1 compared to that of pristine NiCo-LDH (1706.44 F g−1). The hybrid supercapacitors (HSC) assembled using NiCo-3FC and popcorn carbon (PC) achieves a capacitance of 302.19 F g−1 at 1 A g−1 within the voltage range of 1.6 V, outperforming HSC assembled using NiCo-LDH and PC (257.58 F g−1), while exhibiting remarkable enhancement in cycle stability from 54.32 % to 83.63 % after undergoing 5000 cycles. Moreover, it displays a high energy density of 104.57 Wh kg−1 at a low power density of 0.79 kW kg−1, indicating that NiCo-3FC deserves recognition as a high-performance electrode material with significant practical value.