Silk is one of the important collections in the museum, with high cultural, artistic and historical value. As a kind of unstable protein organic material, silk is extremely susceptible to the color damage such as yellowing caused by optical radiation, particularly in the museum light environment where Light Emitting Diode (LED) is widely used. How to evaluate the light-induced color damage to silk scientifically is the main problem to be solved in this study. Although effectively analyzed in the color damage of museum lighting to silk, there is limitations for the color difference evaluation method that is impossible to evaluate the color damage in the induction period. Since the fundamental cause of the color damage to silk lies in the photochemical reaction of the molecular structure inside the material, theoretically, the color damage to silk can be evaluated more scientifically based on Raman spectroscopy, which is studied at the microscopic molecular level. In this study, Raman spectroscopy was introduced into the field of museum lighting to verify its feasibility and scientificity in the color damage evaluation by comparing the evaluation results of the color difference method. Four narrow-band lights at 450, 510, 583, and 650 nm peak wavelengths that constitute the four-primary LED were used to carry out the long-period illumination experiment on silk samples. The relative color damage coefficients of four narrow-band lights on silk samples based on two evaluation methods of color difference and Raman spectroscopy were calculated, which were 450 nm:510 nm:583 nm:650 nm=1.00:0.63:0.48:0.32, and 450 nm:510 nm:583 nm:650 nm=1.00:0.69:0.47:0.27, respectively. On the one hand, the results show that the color damage trend of four narrow-band lights obtained by two methods is consistent, that is, the shorter the peak wavelength, the higher the color damage to silk samples, indicating that Raman spectroscopy is a feasible method to evaluate the light-induced color damage to the silk. On the other hand, the ratio difference of the coefficient obtained based on Raman spectroscopy is greater. There is an induction period in the aging process of silk samples. It is difficult to analyze the change during the induction period by the method of color difference, while the change of molecular structure, including in the induction period, can be detected sensitively by Raman spectroscopy to evaluate the light-induced color damage to silk samples more scientifically. At the same time, the relative color damage coefficients provide a basis for the light-induced color damage evaluation and museum admission evaluation of the four-primary light-emitting diode in the illumination of silk.