Pre-lithiation methods using lithium vanadium fluorophosphate (e.g., LiVPO4F and its derivatives) (“LVPF”) as a cathode active material in a lithium-ion secondary battery. The pre-lithiation methods include compensating for an expected loss of active lithium by selecting LVPF having a specific pre-lithiated chemistry (or a blend of LVPF selected to have a specific pre-lithiated chemistry) and selecting a total amount of the pre-lithiated LVPF. The pre-lithiation methods may include initially charging the lithium-ion secondary battery at the lower of the two charge/discharge plateaus of LVPF to release active lithium.