The invention discloses a method for growing a single-layer graphene thin film by virtue of low-temperature chemical vapor deposition, and belongs to the technical field of two-dimensional thin film material preparation. The preparation method comprises the following steps: (1) preparing an alloy substrate; (2) performing leveling treatment on the alloy substrate; (3) performing annealing treatment on the alloy substrate under a protective atmosphere; and (4) depositing graphene by using a chemical vapor deposition process, and cooling to room temperature to obtain the alloy substrate with a grown single-layer graphene thin film, wherein conditions of the chemical vapor deposition process are as follows: the temperature is 200-800 DEG C, the time is 5-180min, and a carbon source is a gas phase carbon source, a liquid phase carbon source or a solid phase carbon source. The method disclosed by the invention has the advantages that the method is simple, convenient and fast, also is low in cost, and ensures that uniform and single-layer high-quality graphene can be prepared at relatively low temperature; and the method has universality, is simple and mild in condition, uniform in product distribution and good in repeatability, is suitable for industrial production, and is particularly suitable for controllable preparation of single-layer or few-layer graphene.