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• Sustainable way of storing energy with an emphasis on value chain. • Reuse of cotton waste into new active electrode battery materials. • Flexible, self-standing and current collector-free electrode fabrication by pyrolysis. • Long-term cycling of binder-free anodes in Li cells at a high rate. • Stable cycling at various C-rates in lab-scale Li-ion cells with LFP cathode. In this study, self-standing and flexible Li-ion battery negative electrodes made of interconnected two-dimensional carbonized cotton fibers are developed by using a controlled pyrolysis method, and their electrochemical performance in laboratory-scale lithium-based cells is investigated at ambient temperature. By applying this binder- and current collector-free cotton-based carbon fiber electrode, both the Li+-ion intercalation and capacity decay mechanisms are explored using conventional organic carbonate-based liquid electrolyte. The cotton-based carbon fiber electrode shows excellent cycling performance and delivers a high discharge capacity in the voltage range of 0.02 - 1.2 V. The post cycling analysis of carbon fiber using HR-TEM shows the major SEI layer components formed at the surface of the active fibers during the charge/discharge process. The same electrode is used to assemble a lab-scale Li-ion full cell with high mass loading LiFePO 4 -based composite electrode, which demonstrates excellent cycling stability, high Coulombic efficiency and remarkable rate capability at ambient temperature. Synopsis The tenacity to start a sustainable way of producing/storing energy comes from the reuse of waste into new battery materials: back to value chain. Image, graphical abstract [ABSTRACT FROM AUTHOR]