Because of insufficient adhesivity and mechanical properties, conventional polymeric binders fail to accommodate immense volume changes and maintain interparticle connections upon the repeated charge/discharge processes, especially in high active material loading and thick electrodes. Here, a new water-soluble conductive binder (APA/CNT) composed of carboxylic carbon nanotubes interwoven in flexible membranes of the neutralising product of 6-amino-1-hexanol and commercial poly(acrylic acid) (PAA) is developed. The APA/CNT is expected to form robust conductive and elastic network by means of the esterification reinforced electrostatic/H-bonded self-assembly, in which the continuous conductive skeletons can segregate and grasp active nanoparticles by an efficient and robust “sheet-to-point” bonding mode, which endows the as-fabricated anode and cathode with extraordinary structural and interfacial stability, and enhanced electronic conductivity. The as-constructed Si/C anode exhibits superior cycling stability and a high rate performance even under a high mass loading of 15 mg cm⁻², and achieves a high areal capacity of 7.79 mA h cm⁻², far exceeding those of other binder-based Si/C anodes. Moreover, the as-fabricated full cell also displays enhanced electrochemical behaviour and cycling durability. This simple and easy strategy should give a valuable new way to design a cost-effective, universal yet environmentally friendly binder with dependable adhesiveness for high-performance devices.

Flexible lithium-ion batteries (FLIBs) have rapidly developed as promising energy storage devices for flexible and wearable electronics, owning to the advantages of high energy density, fast charge–discharge, no memory effect and stable cycle performance. Research on flexible electrodes has attracted widespread attention to maintain stable electrochemical function under deformation. Carbon materials are some of the most popular lithium-ion battery (LIB) anode materials owing to their low cost, high conductivity and excellent stability. However, the scaled-up fabrication of flexible electrodes based on carbon-based materials for high-performance FLIBs is still challenging. Herein, the fabrication strategies for FLIBs based on carbon materials such as carbon nanofibers (CNFs), carbon nanotubes (CNTs), graphene, graphdiyne (GDY) and carbon aerogels (CAs) are reviewed in terms of macroscopic electrode material preparation, property optimization and structure design. Furthermore, fabrication strategies and structure design methods for electrodes are proposed to improve energy capacity, cycle stability, conductivity and flexibility of FLIBs. This minireview can offer potential directions for the novel design of flexible carbon-based anodes employed in FLIBs.