Highlights A solvent-free thermoplastic forming processing of graphene materials is invented by polymer intercalation from graphene oxide precursor. The correlation between interlayer spacing and thermoplastic forming capability of polymer-intercalated graphene oxide solid is uncovered. The multi-scale forming of graphene materials from Gaussian curved shapes to surface relief patterns with size precision down to 360 nm is realized. The processing capability is vital for the wide applications of materials to forge structures as-demand. Graphene-based macroscopic materials have shown excellent mechanical and functional properties. However, different from usual polymers and metals, graphene solids exhibit limited deformability and processibility for precise forming. Here, we present a precise thermoplastic forming of graphene materials by polymer intercalation from graphene oxide (GO) precursor. The intercalated polymer enables the thermoplasticity of GO solids by thermally activated motion of polymer chains. We detect a critical minimum containing of intercalated polymer that can expand the interlayer spacing exceeding 1.4 nm to activate thermoplasticity, which becomes the criteria for thermal plastic forming of GO solids. By thermoplastic forming, the flat GO-composite films are forged to Gaussian curved shapes and imprinted to have surface relief patterns with size precision down to 360 nm. The plastic-formed structures maintain the structural integration with outstanding electrical (3.07 × 10 5 S m −1 ) and thermal conductivity (745.65 W m −1  K −1 ) after removal of polymers. The thermoplastic strategy greatly extends the forming capability of GO materials and other layered materials and promises versatile structural designs for more broad applications. Graphical abstract