The paper describes a method to produce functionalized single graphene sheets through thermal exfoliation of graphite oxide. The process involves rapid heating of graphite oxide to split it into individual graphene sheets, with the exfoliation mechanism primarily driven by the thermal expansion of evolved gases like CO2. The topological features of the single sheets, as measured by atomic force microscopy, closely match predictions from first-principles atomistic modeling. Despite graphite oxide being an insulator, the functionalized graphene produced is electrically conducting. The study also highlights the importance of complete oxidation and rapid heating in achieving successful exfoliation, and discusses the structural and functional properties of the graphene sheets, including their potential applications in nanocomposites and other materials.The paper describes a method to produce functionalized single graphene sheets through thermal exfoliation of graphite oxide. The process involves rapid heating of graphite oxide to split it into individual graphene sheets, with the exfoliation mechanism primarily driven by the thermal expansion of evolved gases like CO2. The topological features of the single sheets, as measured by atomic force microscopy, closely match predictions from first-principles atomistic modeling. Despite graphite oxide being an insulator, the functionalized graphene produced is electrically conducting. The study also highlights the importance of complete oxidation and rapid heating in achieving successful exfoliation, and discusses the structural and functional properties of the graphene sheets, including their potential applications in nanocomposites and other materials.