The invention discloses a method for synthesizing sugar-undisturbed alpha-glucan with different tightness degrees in vitro, and belongs to the field of food, medicine and starch sugar production. According to the invention, sugar-undisturbed alpha-glucan (GnG) with a certain molecular weight can be synthesized by taking sucrose as a substrate through an SP-GP-BE three-enzyme method; the looseness degree of an outer side chain of the GnG can be controlled by adjusting the ratio of GP to BE, so that different GnG samples with the particle size within the range of 44-54 nm are obtained; and the looseness degree of GnG molecules is improved along with the increase of the ratio of GP/BE. On the basis of controlling GP/BE, the concentration of maltotriose in a reaction system is adjusted; the molecular weight of GnG is reduced along with the increase of the concentration of maltotriose; and meanwhile, the molecular looseness degree of the GnG is increased. According to the method disclosed by the invention, the looseness degree of the GnG molecules can be adjusted by adjusting the GP/BE ratio or adjusting the concentration of maltotriose.