The invention provides a preparation method of a high-quality wafer-level graphene single crystal. The method comprises the following steps: placing plasma-treated metal foil into a reaction furnace,introducing an inert atmosphere, performing heating to an annealing temperature, introducing hydrogen gas, and performing annealing treatment, wherein the metal foil is one selected from the group consisting of copper foil, nickel foil, molybdenum foil and cobalt foil, the plasma treatment atmosphere is at least one selected from the group consisting of air, hydrogen gas, argon gas, oxygen gas, and nitrogen gas, the power is 100-150 W, the pressure is 400-500 Pa, and the time is 1-30 min; and introducing a carbon source into the reaction furnace, adjusting the annealing temperature to a growthtemperature of the graphene single crystal, starting growth of the graphene single crystal, and after growth is completed, performing cooling to a room temperature.