Graphene has been extensively investigated as a host material for Li metal anodes owing to its light weight, high electrical conductivity, high surface area, and exceptional mechanical rigidity. Many studies have focused on assembling twodimensional (2D) graphene sheets into three-dimensional (3D) forms, such as lamination, spheres, and carbon nanotubes; however, little attention has been paid to the technology of modifying 2D graphene sheets. Herein, nanoperforated graphene (NPG) was fabricated through a relatively straightforward process employing metal oxide catalysts based on aqueous solutions. Nanoperforations exhibited a size of approximately 5 nm and were introduced on the graphene sheet and lithiophilic carbonyl groups (C = O) at the edges, facilitating the rapid diffusion of Li+ and lowering the Li nucleation overpotential. In comparison to the reduced graphene oxide (RGO) host, the NPG host exhibited a lower lithium nucleation overpotential and a stable overpotential of ~ 30 mV for over 150 cycles as a stable host structure as a Li metal anode for Li metal batteries.