Lithium-ion batteries are the favored option for portable devices, power tools, and hybrid/full electric automobiles. The latest developments in lithium-ion batteries (LIBs) have yet to fully meet the energy needs for electric vehicle (EV) applications due to their low energy density, despite the continuous evolution of the sector. Silicon is a viable contender for increasing energy density owing to its extraordinary theoretical capacity. However, the enormous increase in size of silicon anodes, growing 2-3 times when absorbing lithium ions, causes pulverization and disrupts electrical contact in the electrode material, leading to severe capacity deterioration. Prior research has proven that strategies like an effective assembly of Silicon/ Graphene via air-controlled electrospray can be utilized to overcome this issue. In addition, the need for a sustainable metal supply-chain calls for prioritizing the use of recycled raw materials over newly mined materials for battery manufacturing. The objective of this work was to explore the feasibility of using recycled Silicon (Si) and Graphene (Gr) hybrid material into LIB anodes as an attempt towards a closed-loop battery value chain. The study investigates the effect of various surface treatments on optimizing the morphology of silicon, combined with graphene obtained from different graphite precursors. An in-depth study of coulombic efficiency, capacity retention, and postmortem analysis revealed that traditional anodes in LIBs could be successfully replaced with recycled Si/Gr anodes without compromising the battery performance.