The invention provides a polypeptide compound for removing wrinkles in eyes. The polypeptide compound, in percentage by mass, consists of the following components: 0.02-0.035% of acetyl hexapeptide-3, 0.001-0.01% of palmitoyl pentapeptide-3, 0.025-0.035% of palmitoyl tetrapeptide-7, 0.025-0.035% of tripeptide, 0.08-0.12% of dipeptide-2, 0.1-0.2% of acetyl tetrapeptide-5, 4-6% of glycerol, 0.2-0.4% of sodium hyaluronate, 0.3-0.5% of 1,2-hexanediol and the balance of purified water. Correspondingly, the invention also provides a preparation method of the compound. The polypeptide compound for removing wrinkles in eyes provided by the invention, applied to volunteers, is capable of taking a significant effect of relieving wrinkles in eyes, so that the average quantity of the wrinkles in eyes is reduced, the depth of the wrinkles in eyes is reduced, the smoothness of eye skin is enhanced, the coverage area of the wrinkles in eyes is reduced and the phenomenon of the wrinkles in eyes is significantly improved.