A supercapacitor features high power density and long cycling life. However, its energy density is low. To ensemble a supercapacitor with high power- and energy-densities, the applied capacitor electrodes play the key roles. Herein, a high-performance capacitive electrode is designed and grown on a flexible carbon cloth (CC) substrate via a hydrothermal reaction and a subsequent ion exchange sulfuration process. It has a 3D heterostructure, consisting of sulfur-doped NiMn-layered double hydroxide (LDH) nanosheets (NMLS) and sulfur-doped NiCo-LDH nanowires (NCLS). The electrode with sheet-shaped NMLS and wire-shaped NCLS on their top (NMLS@NCLS/CC) increases the available surface area, providing more pseudocapacitive sites. It exhibits a gravimetric capacity of 555.2 C g