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Growth of single‐domain GaAs (100) layers on double‐domain Si (100) substrates by molecular beam epitaxy has been investigated. It has been shown that domain orientation of the top layer of GaAs depends on the surface structure of a buffer layer. The size of atomic step heights on the Si surface and the As‐Si interaction temperature before film growth are not important factors in controlling domain orientation. Suppression of an antiphase disorder is explained in terms of nonstoichiometric antiphase boundary annihilation operative during growth.