We have developed a facile one-step hydrothermal strategy to synthesize pyramid-like NiSe2 nanostructures, serving as electrode materials for battery-supercapacitor hybrid (BSH) devices. The NiSe2 nanopyramid electrode exhibits superior electrochemical performances, including a high specific capacity of 240.83 mAh g(-1) at current density of 1 A g(-1) and a low internal resistance of 0.85 . The all-solid-state hybrid devices have been assembled with NiSe2 as the battery-type electrode and activated carbon as the capacitor-type electrode. The hybrid device exhibits a high energy density of 0.196 mWh cm(-2) at power density of 1.60 mW cm(-2). The internal resistance of 1.52 further reveals the nature of low resistance and high conductivity for the hybrid devices. Connecting two hybrid devices in series is able to drive a red LED for more than 3min after charging for 9s. This work has demonstrated that the pyramid-like NiSe2 nanostructure is expected to be an ideal high specific capacity electrode for BSH devices, especially for all-solid-state energy storage devices and portable electronic devices.