Zinc-cobalt double-metal sulfides (ZCS) as Faradic electrode materials with high energy density have great potential fors upercapacitors, but their poor transfer efficiency for electrons and ions hinders their electrochemical response.H erein, ZnCo 2 (CO 3 ) 1.5 (OH) 3 @ZCS microflower hybrid arrays consisting of thin nanolayer petals were anchored on three-dimensional graphene (ZnCo 2 (CO 3 ) 1.5 (OH) 3 @ZCS/3DG) by as imple hydrothermal method and additional ion-exchangep rocess. AZ nCo 2 (CO 3 ) 1.5 (OH) 3 @ZCS/3DG electrode delivered high capacitance (2228 Fg À1 at 1Ag À1 )a nd long cycling life (85.7 %r etention after 17 000 cycles), which are ascribedt ot he multicomponents tructural design. The 3DGconductive substrate improves the electron-transfer dynamics of the electrode material. Meanwhile, the microflowers consisting of thin nanolayer petals could not only provide many actives ites for ions to improve thec apacitance, but also alleviate the volumee xpansion to ensure the structural stability. Furthermore,a na ll-solid-state asymmetric supercapacitor based on aZ nCo 2 (CO 3 ) 1.5 (OH) 3 @ZCS/3DG electrode achieved ah igh energy density of 27 Whkg À1 at 528.3 Wkg À1 ande xhibits exceptional cyclic stability for 23 000 cycles. Its ability to light ab lue LED for 9min verified the feasibility of its applicationf or energy storagedevices.[a] Q. Figure 3. a) XRD pattern of ZnCo 2 (CO 3 ) 1.5 (OH) 3 @ZCS powder,b)Raman spectrum of ZnCo 2 (CO 3 ) 1.5 (OH) 3 @ZCS/3DG,c )XPS full spectrum of ZnCo 2 (CO 3 ) 1.5 (OH) 3 @ZCS/3DG,d -f) Zn 2p, Co 2p, and S2 ph igh-resolution XPS spectra, respectively.