Herein, a crystalline nano-flowers structured zinc oxide (ZnO) was directly grown on carbon fiber textile (CFT) substrate via a simple hydrothermal process and fabricated with a binder-free electrode (denoted as ZnO@CFT) for supercapacitor (SC) utilization. The ZnO@CFT electrode revealed a 201 F·g−1 specific capacitance at 1 A·g−1 with admirable stability of >90% maintained after 3000 cycles at 10 A·g−1. These impressive findings are responsible for the exceedingly open channels for well-organized and efficient diffusion of effective electrolytic conduction via ZnO and CFT. Consequently, accurate and consistent structural and morphological manufacturing engineering is well regarded when increasing electrode materials’ effective surface area and intrinsic electrical conduction capability. The crystalline structure of ZnO nano-flowers could pave the way for low-cost supercapacitors.