AbstractWith the demand for higher energy density and smaller size lithium-ion batteries (LIBs), the development of high specific capacity active materials and the reduction of the usage of inactive materials are the main directions. Herein, a universal method is developed for binder-free electrodes for excellent stable LIBs by rolling the electrospun membrane directly onto the commercial current collector. The rolling process only makes the fiber web denser without changing the fiber structure, and the fiber web still maintains a porous structure. This strategy significantly improves the structural stability of the membrane compared to the direct carbonized electrospun membrane. Moreover, this method is suitable for a variety of polymerizable adhesive polymers, and each polymer can be composited with different polymers, inorganic salts, etc. The electrode prepared by this method can be stably cycled for more than 2000 cycles at a current density of 2500 mA g⁻¹. This study provides a cost-effective and versatile strategy to design the LIB electrode with high energy density and stability for experimental research and practical application.