In this study, we have fabricated helical thin films to be used as an anode material in lithium ion batteries (LIB). The thin films having various CuSi atomic ratios (30–70%, 20–80%, and 10–90%) are prepared by using ion-assisted glancing angle co-deposition.Cu plays a crucial role in holding the electrode together, minimizing overall capacity loss and enabling faster electron transfer thus, improving the electrochemical performances of the electrodes. Increasing the Cu/Si atomic ratio affects the structure of the helices and their alignment. Implementing ion assisted deposition at the beginning of the film deposition helps to improve film adhesion. The Si-20 at.% Cu anode delivers 1885 mAh g−1 initially with 98% coulombic efficiency and retains 77% of the capacity after 100 cycles at 100 mA g−1.