This paper introduces a new design route to fabricate nickel aluminum-layered double hydroxide (NiAl-LDH) nanosheets/hollow carbon nanofibers (CNFs) composite through an in situ growth method. The NiAl-LDH thin layers which grow on hollow carbon nanofibers have an average thickness of 13.6 nm. The galvanostatic charge–discharge test of the NiAl-LDH/CNFs composite yields an impressive specific capacitance of 1613 F g−1 at 1 A g−1 in 6 M KOH solution, the composite shows a remarkable specific capacitance of 1110 F g−1 even at a high current density of 10 A g−1. Furthermore, the composite remains a specific capacitance of 1406 F g−1 after 1000 cycles at 2 A g−1, indicating the composite has excellent high-current capacitive behavior and good cycle stability in compared to pristine NiAl-LDH.