The consumption of lithium has increased dramatically in recent years. This can be primarily attributed to its use in lithium-ion batteries for the operation of hybrid and electric vehicles. Due to its specific properties, lithium will also continue to be an indispensable key component for rechargeable batteries in the next decades. An average lithium-ion battery contains 5–7% of lithium. These values indicate that used rechargeable batteries are a high-quality raw material for lithium recovery. Currently, the feasibility and reasonability of the hydrometallurgical recycling of lithium from spent lithium-ion batteries is still a field of research. This work is intended to compare the classic method of the precipitation of lithium from synthetic and real pregnant leaching liquors gained from spent lithium-ion batteries with sodium carbonate (state of the art) with alternative precipitation agents such as sodium phosphate and potassium phosphate. Furthermore, the correlation of the obtained product to the used type of phosphate is comprised. In addition, the influence of the process temperature (room temperature to boiling point), as well as the stoichiometric factor of the precipitant, is investigated in order to finally enable a statement about an efficient process, its parameter and the main dependencies.