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Currently, with the rise of the photovoltaic industry, how to effectively treat waste silicon powder from an environmentally friendly and economic point of view becomes significant. We reported a simple method to prepare the "core-shell" structure of silicon/carbon nanotubes/carbon (Si/CNTs/C) composite by ball-milling using waste silicon powder. Specifically, The synergistic effect of CNTs and amorphous carbon matrix is beneficial to improving the transmission rate of Li-ions and electrons, and facilitating the reaction kinetics of Li-ions in the process of lithiation/de-lithiation. Meanwhile, the carbon coating layer reduces the direct contact between silicon and the electrolyte, which greatly alleviates the volume expansion of silicon in cycling. With these merits, Si/CNTs/C anode shows high rate performance and outstanding cycling stability up to 300 cycles at 0.2C. Furthermore, full cells assembled with pre-lithiated Si/CNTs/C anodes and commercial NCM811 cathodes deliver considerable initial coulombic efficiency (84.4%) and high energy density (502 Wh kg−1). Si/CNTs/C composites prepared by ball-milling show excellent long-cycle stability and rate performance. [Display omitted] • Industrial waste silicon is used to prepare silicon-based anodes. • Two-step ball milling method to prepare Si/CNTs/C composite. • A solution-based chemical prelithiation method is proposed. • Si/CNTs/C anode exhibits excellent long-cycle stability and good rate performance. • A full cell shows an improved ICE (84.4%) and a higher energy density (502 Wh kg−1). [ABSTRACT FROM AUTHOR]