▎ 摘　　要

Graphene is a fascinating two-dimensional material, but easy restacking and a zero band gap restrict its practical applications. To solve these issues, we designed a new chemical reaction between lithium hydride and CO, achieving a one-step catalyst-free synthesis of hierarchically three-dimensional (3D) hydrogenated graphene (HG) with large specific surface area (up to 494 m(2)/g) and a 1.31 eV band gap. Furthermore, the HG sheet possesses a thickness from 1.01 to 1.31 nm and hydrogenation degree from 18 to 33%, which are dependent on reaction temperature. These findings provide a new approach to develop graphene-based materials with tunable properties.