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Large area (cm2) multi-layer graphene film is synthesized in the substrate-free vapor?phase. The scanning electron microscopy observation reveals that the graphene nanoflakes?are either six- or five-sided, and the internal angles between adjacent sides are nearly 120?and 105, respectively. The nucleation of hexagonal and pentagonal carbon rings leads to?carbonaceous nuclei, which grow into six- or five-sided nanoflakes, respectively. A wellordered?and large-area graphene monolayer is formed by the interconnection of these?flakes, and stacking of these monolayers results in the formation of a multi-layer graphene?film. The creation of hexagonal and pentagonal carbon rings is considered to be important?for the easy production of large area multi-layer graphene at large scale.