With a remarkable theoretical specific capacity of ~4200 mAh g-1, silicon anode is at the forefront to enable lithium-ion batteries (LIBs) with ultra-high energy density. However, we have yet to...

The demand for high-capacity lithium-ion batteries (LIBs) is ever-increasing. Thus, research has been focused on developing silicon-based anodes due to their high theoretical capacity and natural abundance. However, silicon-based anodes still suffer from several drawbacks (e.g., a huge volume expansion during lithiation/delithiation and the low conductivity nature of silicon). In this study, we develop a facile and low-cost synthesis route to create a composite of silicon particles and carbon nanotubes (CNTs) via simple two-step mechanical ball milling with a silicon wafer as the silicon precursor. This method produces a strong interaction between silicon particles and the CNTs, forming Si–C bonds with minimum oxidation of silicon and pulverization of the CNTs. The resulting Si/CNT anode exhibits a first cycle Coulombic efficiency of 98.06%. It retains 71.28% of its first cycle capacity of 2470 mAh g−1 after 100 cycles of charge–discharge at a current density of 400 mA g−1. Furthermore, the Si/CNT anode also shows a good rate capability by retaining 80.15%, and 94.56% of its first cycle capacity at a current density of 1000 mA g−1 and when the current density is reduced back to 200 mA g−1, respectively.