A nanoflower structure of Zn[Formula: see text]Co[Formula: see text]S directly grown on carbon fiber papers (CFP) was successfully designed by a mild two-step hydrothermal method. Benefiting from their fascinating structural features, Zn[Formula: see text]Co[Formula: see text]S/CFP electrode exhibits a maximum specific capacitance of 300[Formula: see text]F[Formula: see text]g[Formula: see text] at current density of 1[Formula: see text]A[Formula: see text]g[Formula: see text] and 84% capacitance retention after 5,000 cycles at current density of 5[Formula: see text]A[Formula: see text]g[Formula: see text]. Subsequently, Zn[Formula: see text]Co[Formula: see text]S/CFP//AC all-solid-state asymmetric supercapacitor (ASC) device is assembled and able to illuminate the red LEDs. ASC devices deliver a maximum energy density of 9.59[Formula: see text]W[Formula: see text]h[Formula: see text]kg[Formula: see text] at a power density of 750[Formula: see text]W[Formula: see text]kg[Formula: see text]. Therefore, this impressive result demonstrates that the nanoflower Zn[Formula: see text]Co[Formula: see text]S have promising applications in the development of high-performance supercapacitors.