Two-dimensional (2D) multilayered graphitic carbon nanosheets are prepared via a facile, green, and mild method of one-pot hydrothermal carbonization at a temperature below 300 °C. Copper with a 2D structure is formed in situ and serves as both a template and catalyst. The obtained multilayered carbon nanosheets exhibit well-defined shapes and a radius-to-thickness ratio as high as 104, with monolayer thickness as small as 2.86 nm.