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As an outstanding kind of flexible energy conversion device, flexible solid-state supercapacitors (FSSCs) show enormous advantages in flexible, portable, and wearable devices. The performance improvement of flexible electrodes shows a significant role in constructing high-performance FSSCs. Herein, the polyaniline (PANI) nanowire array on the surface of carbon cloth (CC) is utilized to assist the surface oxidation of CC, and the unique surface treatment process aims to improve the specific surface area and provides an abundance of heteroatoms to increase the storage of charge for high electrochemical performance. As a result, the obtained PANI nanowire array-assisted surface oxidation of CC (AOCC) exhibits optimal area capacitance (1614 mF/cm2), high rate capability (63.1% even up to 100 mA/cm2), and excellent cycling stability (105% of the original value even up to 20 000 cycles). Furthermore, flexible AOCC electrodes are explored for constructing FSSC devices, which possess high energy density (0.51 mW h/cm3) and power density (68.6 mW/cm3) and extremely good cycling stability (maintaining 93.3% of initial capacitance value after 10 000 cycles). In addition, the FSSCs demonstrate superior mechanical performances and flexibility. Therefore, AOCC is expected to be a high-performance flexible electrode in FSSCs.