A hierarchical core-shell heterostructure comprised of vertical and intercrossing ultrathin NiMn-LDHs nanosheets shell and slightly curly and tops tangled CuO nanowires core shows promising electrochemical storage properties. Display omitted •A hierarchical NiMn-LDH@CuO/CF core-shell heterostructure was successfully prepared.•The hybrid comprises of vertical NiMn-LDHs shell and tops tangled CuO nanowires core.•The NiMn-LDH@CuO/CF electrode exhibits high capacitance of 6077 mF cm−2 at 2 mA cm−2.•The blue LED indicator can be lit up eight minutes by three ASCs connected in series. Supercapacitors are attracting tremendous research interest because they are expected to achieve battery-level energy density while having long calendar life and short charging time. Ultrathin layered double hydroxide nanosheets (LDHs) are promising candidates as electrode materials for energy storage. Herein, we have successfully designed and synthesized a hierarchical NiMn-LDH@CuO/CF core-shell heterostructure which comprises a vertical and intercrossing ultrathin NiMn-LDHs nanosheets shell and a slightly curly and tops tangled CuO nanowires core. The synthesized NiMn-LDH@CuO/CF electrode exhibits a high areal capacitance of 6077 mF cm−2 (2430.8 F g−1) at a current density of 2 mA cm−2 (0.8 A g−1), which is significant higher than those of CF, Cu(OH)2/CF, CuO/CF, NiMn-LDH/CF and NiMn-LDH electrodes. Moreover, a superior cycling stability of 89.22% retention after 8000 cycles at a high current density of 50 mA cm−2 is observed and a low internal resistance Rs (0.584 Ω) can be achieved. Furthermore, an all solid-state asymmetric supercapacitor (ASC) device based on the as-synthesized hierarchical NiMn-LDH@CuO/CF core-shell heterostructure hybrid material as positive electrode and activated carbon as negative electrode is successfully fabricated and exhibits an energy density of 10.8 W h kg−1 at a power density of 100 W kg−1. Additionally, a LED indicator can be lit up for eight minutes when three ASCs are connected in series. The excellent electrochemical performances can be credited to the significant enhancement of the specific surface area, charge transport and mechanical stability resulted from the ultrathin LDH shell, the highly conductive CuO nanowires core-shell nanostructure. This strategy for the fabrication of hierarchical core-shell heterostructure could have enormous potential for applications in high performance energy storage devices.