It is challenging to efficiently and economically recycle many lithium-ion batteries (LIBs) because of the low valuation of commodity metals and materials, such as LiFePO4. There are millions of tons of spent LIBs where the barrier to recycling is economical, and to make recycling more feasible, it is required that the value of the processed recycled material exceeds the value of raw commodity materials. The presented research illustrates improved profitability and economics for recycling spent LIBs by utilizing the surplus energy in lithiated graphite to drive the preparation of organolithiums to add value to the recycled lithium materials. This study methodology demonstrates that the surplus energy of lithiated graphite obtained from spent LIBs can be utilized to prepare high-value organolithiums, thereby significantly improving the economic profitability of LIB recycling. Organolithiums (R–O–Li and R–Li) were prepared using alkyl alcohol (R–OH) and alkyl bromide (R–Br) as substrates, where R includes varying hindered alkyl hydrocarbons. The organolithiums extracted from per kilogram of recycled LIBs can increase the economic value between $29.5 and $226.5 kg−1 cell. The value of the organolithiums is at least 5.4 times the total theoretical value of spent materials, improving the profitability of recycling LIBs over traditional pyrometallurgical ($0.86 kg−1 cell), hydrometallurgical ($1.00 kg−1 cell), and physical direct recycling methods ($5.40 kg−1 cell).