A method for adjusting and controlling a boundary of graphene, comprising: providing an insulating substrate and placing the insulating substrate in a growth chamber; and feeding first reaction gas into the growth chamber, the first reaction gas at least comprising carbon source gas, and controlling a flow rate of the first reaction gas to forming a graphene structure having a first boundary shape on a surface of the insulating substrate through controlling a flow rate of the first reaction gas. The present invention realizes the controllability of the boundary of the graphene by adjusting the ratio of the carbon source gas to catalytic gas in the growth process of graphene on the surface of the substrate; the present invention can enable graphene to sequentially continuously grow by changing growth conditions on the basis of already formed graphene, so as to change the original boundary shape of the graphene.