An easy novel approach which offers a fast pathway of macroscopic quantity preparation of graphene nanosheets (GS) at room temperature has been firstly proposed via lithium aluminum tetrahydride (LiAlH 4 ) and phosphorus tribromide (PBr 3 ) as the deoxidizer based on graphite oxide (GO). The structure of the graphene was investigated by high-resolution transmission electron microscopy (HR-TEM) indicating the GS with few layers (~3 layers). It is found that the GS as anode material used for lithium ion battery (LIB) has high initial coulombic efficiency (83.1%). The first discharge and charge capacity of the prepared GS were 1029.4mAh·g −1 and 855.1mAh·g −1 at a current density of 100mA·g −1 , respectively. After 21cycles, the reversible capacity is still kept at 760.7mAh·g −1 . The as-prepared GS with few layers and defects could be optimized for excellent electrochemical performance as lithium ion battery anode material.