The annealing of graphene layers grown on 150 nm thick single crystal Ni(111) films was investigated in situ by low energy electron microscopy and photoemission electron microscopy. After growth, by means of chemical vapor deposition of ethylene, the graphene layers consist of several domains showing different orientations with respect to the underlying Ni surface and also of small bilayer areas. It is shown that, in a controlled process, the rotated domains can be transformed into lattice-aligned graphene, and the bilayer areas can be selectively dissolved, so that exclusively the aligned monolayer graphene is obtained. The ordering mechanism involves transport of C atoms across the surface and solution in the bulk.

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