To improve the reversible capacity and electrochemical performance of the Li-ion batteries, prelithiation is one of the promising solutions as it leads to the reduction of irreversible capacity and stabilization of electrode surfaces after prelithiation. However, typical electrochemical prelithiation has drawbacks including a longer reaction period and low efficiency of the process. Here, we demonstrate a facile route for the one-pot synthesis of chemically prelithiated graphene before assembling the battery cell. In the reaction of a mixture consisting of graphene oxide (GO), lithium, and 4,4'-di-tert-butylbiphenyl (DTBP), the prelithiation and reduction of GO have occurred simultaneously by the assistance of DTBP. The prelithiated graphene exhibits improved reversible capacity (643 mAh g(-1)), cyclic stability (capacity retention of 87.4% after 200th cycle), and rate capability compared to those of GO and reduced graphene oxide (RGO). This chemical prelithiation method is expected to enable the efficient production of prelithiated graphene anodes for improving the performance of Li-ion batteries.