mers usually suffer from poor cyclic stability in long term charge-discharge processes. [ 15 ] The low electron conductivity of transition metal oxides leads to inferior rate capability. [ 16 ] In the search for high performance electrode materials, transition-metal sulfi des have been extensively studied as new class of pseudocapacitive materials for supercapacitors. [17][18][19][20] In particular, NiCo 2 S 4 possess higher electrochemical activity and higher capacity than mono-metal sulphides based on richer redox reactions. [ 21,22 ] More signifi cantly, NiCo 2 S 4 exhibited an excellent electrical conductivity, at least two orders of magnitude higher than that of NiCo 2 O 4 . [ 23 ] The development of novel nanostructured materials will effectively improve the utilization of active materials because of their high surface area, and short electron-and ion-transport pathways. Several different types of NiCo 2 S 4 nanostructures, including nanoplates, [ 24 ] nanoprisms, [ 25 ] nanotubes, [ 26,27 ] microspheres, [ 28 ] have been recently synthesized and their electrochemical performance was investigated. For example, Lou et al. [ 25 ] reported the fabrication of Ni x Co 3-x S 4 hollow nanoprisms through a simple sacrifi cial template method and a high reversible capacity (895 F g −1 under 1 A g −1 ) can be achieved. However, it should be noted that the introduction of a conductive agent and a polymer binder during the thin fi lm electrode preparation not only increase extra contact resistance but also inevitably compromises the overall energy storage capacity that still seriously limit their performance. [ 29,30 ] Three dimensional (3D) electrode architectures have emerged as a new direction because it can provide 3D interconnected network of both electron and ion pathways, allowing for effi cient charge and mass exchange during faradic redox reactions. Greatly enhanced performance has kindled the interest of researchers in the fi eld of 3D electrode architectures designs, such as copper pillar array, [ 31 ] nickel network, [ 32,33 ] stainless steel mesh, [ 34 ] carbonaceous interpenetrating structures. [ 35 ] The rigid electrode with metals as current collectors lead to the devices less fl exible, and they also have a low energy density. Carbon nanotubes sponge and graphene foams have been recently fabricated using chemical vapor deposition and used as electrode architectures for supercapacitors. [36][37][38] However, it is diffi cult to produce carbonaceous foams in large-scale because of their relatively high-cost and complex preparation processes. Additionally, due to the potential incompatibility issue between To push the energy density limit of supercapacitors, a new class of electrode materials with favorable architectures is strongly needed. Binary metal sulfi des hold great promise as an electrode material for high-performance energy storage devices because they offer higher electrochemical activity and higher capacity than mono-metal sulfi des. Here, the rational design and fabrication of NiCo 2 S 4 nan...