In this work, a facile two-step hydrothermal method was reported to grow hierarchical flower-like NiAl layered double hydroxide (LDH) directly on 3D nickel foam (NF) which was further coated with 2D graphene nanosheets (GNS) layers as binder-free supercapacitor electrode. The positive and negative effects of GNS on the electrochemical performance of LDH-NF electrode were investigated in detail. The prepared LDH-NF/GNS electrode maintained an enhanced specific capacity of 165.6 C g⁻¹ after 4000 cycles at a high current density of 40 A g⁻¹. Furthermore, a hybrid supercapacitor, with LDH-NF/GNS and GNS-NF as the positive and negative electrodes, achieved an energy density (31.5 Wh kg⁻¹ at a power density of 400 W kg⁻¹) and super long-term cycle stability (a specific capacity of 67.2 C g⁻¹ at 5 A g⁻¹ after 5000 cycles with 80% retention). This study not only opens up the possibility of engineering LDH-NF/GNS into a promising electrode, but also highlights the positive and negative roles of GNS on LDH-NF as binder-free electrodes for further development of high-performance supercapacitors.