AbstractSelf‐supported hollow nanoarrays with rich active sites hold great promise as binder‐free electrode for supercapacitors. In this work, the hollow Co‐Ni−S nanowedge arrays (NWAs) have been fabricated on Ni foam (NF) substrate through a facile sulfidation and etch of ZIF−L‐Co NWAs/NF. Structural evolution upon solvothermal time indicates that the formation of hollow Co‐Ni−S NWAs is mainly due to the etch of defect‐rich interior of solid ZIF−L‐Co NWAs. The unique hollow nanowedge structural and compositional advantages ensure the hollow Co‐Ni−S NWAs excellent electrochemical properties with areal capacity of 0.286 mA h cm−2 at 5 mA cm−2, and 78% capacity retention after 2000 cycles. Moreover, the hybrid supercapacitor (HSC) of Co‐Ni−S // AC has been assembled, which illustrates good application performance. The results indicate that the Co‐Ni−S NWAs/NF is a promising binder‐free electrode for high‐performance hybrid supercapacitors.