Hierarchical Ni0.54Co0.46O2 architectures composed by nanowires or nanosheets were successfully grown on bio-mass carbon fiber cloth (CFC) by hydrothermal method. The morphology of Ni0.54Co0.46O2 can be effectively controlled by using different precipitators. The structural effects of the two kinds of morphologies were researched. the results suggest that the Ni0.54Co0.46O2 nanosheet arrays grown on CFC (NCO-NSs/CFC) shows a higher Faradaic areal capacity of 438 μAh cm−2 (238.1 mAh g−1) at a current density of 1 mA cm−2 and still about 90.3% initial capacity retention even at the high current density of 50 mA cm−2. Moreover, an all-solid-state flexible symmetric supercapacitor device has been successfully assembled. The optimized device delivers superior electrochemical performance with an outstanding energy density of 92.4 Wh kg−1 at a power density of 207.2 W kg−1. Such hierarchical nanostructure composed by well-aligned uniform Ni0.54Co0.46O2 nanosheet arrays grown on bio-mass carbon fiber cloth might hold great promise as battery-type electrode material for high-performance supercapacitor.