Energy storage devices like batteries and supercapacitors, have become indispensable in portable devices and electric vehicles. But, the carbon anodes used in these devices, exhibit a significant loss in their initial capacity (graphite: 6.6% and hard carbon: 29.8%) due to the consumption of Li ions from electrolyte during solid electrolyte interface layer formation and other non-reversible reactions, and if unaddressed, can potentially diminish this advantage. Pre-lithiation treatment of carbon anodes can mitigate this loss, apart from improving the cell working potential, hence enhancing cell energy density and cyclability. We investigate in this report a direct-contact lithiation process in graphite and hard carbon anodes using four distinct lithium source structures. The results show that the type of Li-source structure employed for anode pre-lithiation can have a major impact on the electrode physical properties, pre-lithiation times and the pre-lithiation anode potentials achieved, potentially effecting the SEI properties, cycle life, and the electrode processing costs. for their reversible characteristic, where a guest ion (e.g. Li-ion) can be reversibly intercalated and de-intercalated into the host carbon material. On the other hand, the host carbon anode materials when in contact with organic electrolytes (Li salt in organic solvents), form an electronically passivating solid electrolyte interface (SEI) layer 3 on their surface by the reduction of electrolyte. This ensures the longterm stability of the device by passivating the carbon anode surface by preventing further reduction of the electrolyte on the anode surface. This SEI layer is ionically conductive enough to provide Li-ion pathways passing through it for further intercalation into the bulk of anode after de-solvating them, therefore preventing the co-intercalation of solvent molecules into the carbon structure. Although, the formation of SEI layer is necessary and beneficial, nevertheless, it consumes the Li-ions from the electrolyte, depleting it of charge carriers. This is the initial irreversible cycle loss 4 and if not compensated for, then it can drastically affect the efficiency and cyclability of the energy storage device. 5 The initial cycle loss can be mitigated by supplying additional Li-ions from Li reservoirs and this process is generally known as pre-lithiation. Apart from mitigating the initial cycle loss, pre-lithiation also improves the working potential of the device by providing a lower redox potential to the carbon anode, hence raising the overall cell potential, which further results into higher cell energy density, cycle stability and reduced electrode resistance. 2,6 Moreover, due to the pre-lithiation process, the anion-cation concentration in the electrolyte remains mostly stable during cycling, hence maintaining a steady electrolyte conductivity, which is crucial for cell efficiency and cyclability.Pre-lithiation can be achieved through several methods, 7 including electrochemically driven lithiation, 8 lithiation usi...