This paper presents the synthesis, structure, and properties of boron (B) and nitrogen (N)-doped graphene. The authors prepared B- and N-doped graphene bilayer samples using different methods, including arc discharge and transformation of nanodiamonds, and investigated their structure and properties. First-principles DFT calculations were performed to understand the effects of substitutional doping on the structure and electronic and vibrational properties of graphene. The synthesis of B-doped graphene (BG) was achieved through two methods: arc discharge of graphite electrodes in the presence of H₂ + B₂H₆ (BG1) and arc discharge using a boron-stuffed graphite electrode (BG2). Nitrogen-doped graphene (NG) was prepared by arc discharge in the presence of H₂ + pyridine (NG1), H₂ + ammonia (NG2), and transformation of nanodiamonds in the presence of pyridine (NG3). All samples were characterized using various physical methods, including XPS, EELS, XRD, TEM, AFM, and TGA. XPS and EELS analysis showed that BG1 and BG2 contained 1.2 and 3.1 at% boron, respectively, while NG1, NG2, and NG3 contained 0.6, 0.9, and 1.4 at% nitrogen, respectively. XRD and TEM images confirmed that the samples contained 2-3 layers on average. TGA showed that B- and N-doped samples underwent combustion at a slightly lower temperature than pure graphene (580 °C). Raman spectroscopy revealed that the G band stiffens with both B and N doping, similar to electrochemical doping. The intensity of the D band was higher than that of the G band in all doped samples, and the relative intensity of the 2D band generally decreased with doping. The in-plane crystallite sizes of the samples were calculated using the formula: La(nm) = (2.4 × 10⁻¹⁰)λ⁴(ID/IG)⁻¹. The crystallite sizes of the samples were found to be smaller than that of undoped graphene. The authors also performed DFT calculations to study the electronic structure and vibrational properties of B- and N-doped graphene. The results showed that B-doped graphene has a smaller band gap and a weaker quadratic dispersion compared to N-doped graphene. The Fermi energy was shifted by -0.65 eV and 0.59 eV for 2 at% B and N substitutions, respectively, resulting in p-type and n-type semiconductor behavior. The study demonstrates that B- and N-doped graphene can be synthesized to exhibit p- and n-type semiconducting electronic properties, which can be systematically tuned with the concentration of B and N. Raman spectroscopy of the G- and DThis paper presents the synthesis, structure, and properties of boron (B) and nitrogen (N)-doped graphene. The authors prepared B- and N-doped graphene bilayer samples using different methods, including arc discharge and transformation of nanodiamonds, and investigated their structure and properties. First-principles DFT calculations were performed to understand the effects of substitutional doping on the structure and electronic and vibrational properties of graphene. The synthesis of B-doped graphene (BG) was achieved through two methods: arc discharge of graphite electrodes in the presence of H₂ + B₂H₆ (BG1) and arc discharge using a boron-stuffed graphite electrode (BG2). Nitrogen-doped graphene (NG) was prepared by arc discharge in the presence of H₂ + pyridine (NG1), H₂ + ammonia (NG2), and transformation of nanodiamonds in the presence of pyridine (NG3). All samples were characterized using various physical methods, including XPS, EELS, XRD, TEM, AFM, and TGA. XPS and EELS analysis showed that BG1 and BG2 contained 1.2 and 3.1 at% boron, respectively, while NG1, NG2, and NG3 contained 0.6, 0.9, and 1.4 at% nitrogen, respectively. XRD and TEM images confirmed that the samples contained 2-3 layers on average. TGA showed that B- and N-doped samples underwent combustion at a slightly lower temperature than pure graphene (580 °C). Raman spectroscopy revealed that the G band stiffens with both B and N doping, similar to electrochemical doping. The intensity of the D band was higher than that of the G band in all doped samples, and the relative intensity of the 2D band generally decreased with doping. The in-plane crystallite sizes of the samples were calculated using the formula: La(nm) = (2.4 × 10⁻¹⁰)λ⁴(ID/IG)⁻¹. The crystallite sizes of the samples were found to be smaller than that of undoped graphene. The authors also performed DFT calculations to study the electronic structure and vibrational properties of B- and N-doped graphene. The results showed that B-doped graphene has a smaller band gap and a weaker quadratic dispersion compared to N-doped graphene. The Fermi energy was shifted by -0.65 eV and 0.59 eV for 2 at% B and N substitutions, respectively, resulting in p-type and n-type semiconductor behavior. The study demonstrates that B- and N-doped graphene can be synthesized to exhibit p- and n-type semiconducting electronic properties, which can be systematically tuned with the concentration of B and N. Raman spectroscopy of the G- and D