The study presents a method for the simultaneous nitrogen-doping and reduction of graphene oxide (GO) sheets through thermal annealing in ammonia (NH₃). X-ray photoelectron spectroscopy (XPS) analysis reveals that N-doping occurs at temperatures as low as 300°C, with the highest doping level of ~5% N achieved at 500°C. The reduction of GO is accompanied by a decrease in oxygen levels from ~28% in as-made GO to ~2% in NH₃-reacted GO at 1100°C. XPS analysis shows the presence of pyridinic N in the doped samples, with increased quaternary N (N that replaces carbon atoms in the graphene plane) in samples annealed at higher temperatures (>900°C). Oxygen groups in GO are responsible for reactions with NH₃ and C-N bond formation. Pre-reduced GO with fewer oxygen groups exhibits reduced reactivity with NH₃ and lower N-doping levels. Electrical measurements of individual GO sheet devices demonstrate that GO annealed in NH₃ exhibits higher conductivity than those annealed in H₂, suggesting more effective reduction by NH₃. The N-doped reduced GO shows n-type electron doping behavior with a Dirac point at negative gate voltages in three-terminal devices. The method provides a route for the synthesis of bulk amounts of N-doped, reduced GO sheets, which could have useful properties for various applications.The study presents a method for the simultaneous nitrogen-doping and reduction of graphene oxide (GO) sheets through thermal annealing in ammonia (NH₃). X-ray photoelectron spectroscopy (XPS) analysis reveals that N-doping occurs at temperatures as low as 300°C, with the highest doping level of ~5% N achieved at 500°C. The reduction of GO is accompanied by a decrease in oxygen levels from ~28% in as-made GO to ~2% in NH₃-reacted GO at 1100°C. XPS analysis shows the presence of pyridinic N in the doped samples, with increased quaternary N (N that replaces carbon atoms in the graphene plane) in samples annealed at higher temperatures (>900°C). Oxygen groups in GO are responsible for reactions with NH₃ and C-N bond formation. Pre-reduced GO with fewer oxygen groups exhibits reduced reactivity with NH₃ and lower N-doping levels. Electrical measurements of individual GO sheet devices demonstrate that GO annealed in NH₃ exhibits higher conductivity than those annealed in H₂, suggesting more effective reduction by NH₃. The N-doped reduced GO shows n-type electron doping behavior with a Dirac point at negative gate voltages in three-terminal devices. The method provides a route for the synthesis of bulk amounts of N-doped, reduced GO sheets, which could have useful properties for various applications.