Nickel-based layered hydroxides (LDHs) have aroused much interest as promising battery-type electrodes for hybrid supercapacitors (HSCs) because of their high theoretical capacity, good safety, and abundant natural resources; however, the electrochemical performances are still notoriously limited owing to their intrinsically poor electrical conductivity and severe agglomeration features. Herein, an elaborate hierarchical NiCo2S4@NiCu-LDH nanotube/nanosheet hybrid electrode is designed and fabricated directly on carbon cloth by a facile multistep solution-based strategy. Through the rational engineering of nanostructures and atomic substitution of nickel by copper, the optimized NiCo2S4@NiCu-LDH hybrid electrode can yield a high areal capacity of 632.0 mu Ah/cm(2) at a current density of 2 mA/cm(2) and a good rate capability. Furthermore, the assembled flexible solid-state HSC device employing the NiCo2S4@NiCu-LDH exhibits a maximum volumetric energy density of 2.7 mWh/cm(3) at a power density of 21.3 mW/cm(3) with a robust long-term cycling stability over 2000 cycles and outstanding flexibility under repeated bending tests. Our work demonstrates the possibility of designing and fabricating nickel-based LDHs as superior battery-type electrodes towards highly durable and efficient flexible energy storage devices.