AbstractChemically modified graphene was synthesized by chemical vapour deposition (CVD) with ammonia gas introduced during the CVD process. The use of two different metal catalyst films [nickel (Ni) or copper (Cu)] results in distinctly different forms of structural defects in the honeycomb lattice of graphene under identical synthesis conditions. The Ni catalyst film gave rise to numerous “flower‐like” defects, where carbon atoms formed core hexagons surrounded by pentagons alternated with heptagons, whilst graphene grown on a Cu catalyst film contained a much higher concentration of substituted nitrogen atoms. The samples were characterized by a variety of spectroscopic and microscopic methods complemented with electrical transport measurements.magnified image