The invention provides a method for preparing high-carbon hydrocarbons from methane through vacuum ultraviolet radiation. Major equipment comprises a methane storage tank, a refining system, an argon gas storage tank, a blender and a plurality of series vacuum ultraviolet radiation reactors, wherein the high-carbon hydrocarbons are separated from a product flowing out of a last-stage reactor by a primary condenser, and uncondensed gas mixture is pumped back; hydrogen gas produced by a reaction is subjected to recovery by a hydrogen-pervious palladium membrane separator and a hydrogen gas vacuum pump and then is pumped into fuel cells for power generation, the high-carbon hydrocarbons are recovered from impervious methane, ethane, propane, butane and pentane by a condenser and a gas-liquid separator, and then, uncondensed gas returns to a system. According to the method, multistage vacuum ultraviolet radiation reactions are adopted, the byproduct hydrogen gas is recovered, and the high-carbon hydrocarbons are subjected to primary separation, so that the dehydrogenation of the methane and the production of alkanes are promoted; the alkanes are circularly applied mechanically as a reaction assistant of the methane and an initiator of optical free radical chains, so that the efficiency of photo-induced reaction is increased, the conversion ratio of the methane and the product yield are increased, and the production cost of the high-carbon hydrocarbons is reduced.