“…With the rapid development of wearable electronics, energy-storage devices have gained much attention because of their high flexibility, light weight, and good electrochemical properties. − Among them, a lot of researchers have paid close attention to the flexible supercapacitors because of their higher energy density, long life cycle, and an extensive applicable temperature range. , Accordingly, many efforts recently have been focused on endowing flexible supercapacitors with higher efficiency, better cycling stability, and lower cost in order to achieve fully self-supporting flexible electronics. − As a kind of natural, renewable biomass nanomaterial, cellulose nanofibers (CNFs) show great potential for fabricating electrode materials as an ideal binder and building blocks derived from its high hydrophilicity, large specific surface area, excellent mechanical properties, and charged surface with a lot of carboxyl groups. , As a matter of fact, a lot of research proved that it is an outstanding material for preparing flexible supercapacitors. , Polypyrrole (PPy) has been frequently employed on energy-storage devices such as electrode materials because of its large specific capacitance (>600 F g –1 ), good electrical conductivity, and environmental stability. − However, it displays unsatisfactory cycling stability during electrochemical processes because of the sustained volume expansion and contraction of PPy during continuous redox processes. Therefore, graphene, carbon nanotubes (CNTs), and their derivatives are frequently used to enhance the capacitance properties of PPy as an electrode for supercapacitors. − One of them, graphene oxide (GO) displayed an effective improvement for the capacitance stability because of its excellent ductility and mechanical properties. − For these reasons, in order to fabricate supercapacitors with flexible, tensile, and high capacitance properties, CNF, graphene, and PPy are integrated regularly to prepare self-supporting flexible electrodes with a two-dimensional thin film or porous materials by different structure design and various fabrication processes. , …”