To explore the application of in-situ Raman spectroscopy for monitoring the curing reaction of energetic materials by using toluene diisocyanate （TDI） as curing agent， both in-situ infrared （IR） and Raman spectroscopy were employed to study the spectral changes before and after the curing reaction of 3，3-bis（azidomethyl）oxetane-tetrahydrofuran co-polyether （PBT）-TDI system. The Raman bands suitable for quantitative monitoring of the curing process were analyzed， and the results were evaluated. The vibrational modes of the Raman bands of reactants and products were identified using density functional theory （DFT） method. The correlation between the curing reaction results obtained from IR and Raman spectroscopy was also discussed. Results show that the peak of 1534 cm^-1 in Raman spectroscopy of the PBT-TDI system exhibits a low signal-to-noise ratio， making it unsuitable for quantitative analysis. The reaction degree calculated from the peak of 1743 cm^-1 in Raman spectroscopy is significantly higher than that derived from the peak of 2269 cm^-1 in IR spectroscopy. The peak of 1505 cm^-1 in Raman spectroscopy is associated with the stretching vibration of the isocyanate （NCO） group. The differences in the degree of reaction is due to the number of individual NCO groups in the TDI molecules participating in the reaction. The two methods show complementary roles in monitoring the curing process.