Silk, a natural protein fiber, is widely used in the textile industry and biomedical materials for its excellent properties. However, its application in some fields is seriously restricted due to its poor anti-wrinkle behavior. In this study, 2,4,6-trichloropyrimidine (TLP) was used in the production of anti-wrinkle silk fabrics. The optimum finishing conditions were as follows: 3-g/L 2,4,6-trichloropyrimidine, 6-g/L NaHCO3, 8-g/L Na2SO4, finishing temperature of 65 °C, and finishing time of 40 min. The crease recovery angle of the finished fabric is 16–20% higher than the unfinished fabric, and the finishing process has a small effect on the whiteness of silk while achieving some degree of washing resistance. The morphology and chemical structures of the finished silk fabric were characterized by scanning electron microscopy and Fourier transform infrared spectroscopy. The K/S value of the finished silk fabric dyed with reactive dyes increased compared with the silk fabric only dyed, indicating that the dyeability of the finished fabric was improved. This technology provides a new method for fabricating silk color crease-resistant fabrics.