The stability of hydrogen-bonded energetic material 3-nitropyrazole (3-NP, C3H3N3O2) under high pressure was studied using a diamond anvil cell, Raman spectrometer, and simulation calculation. Under the hydrostatic experimental pressure and simulated pressure of 10 GPa, the optical Raman spectra, the change of cell parameters, and the Hirshfeld surface energy of 3-NP were obtained respectively. The analysis of the measured Raman spectra shows that the structure is still in original phase at 10 GPa pressure. The effects of pressure on cell parameters, molecular arrangement, and hydrogen bonding were observed by simulation calculation. Systematic analysis of the subtle structural changes, anisotropic characteristics, and various interactions of 3-NP shows that the stability of 3-NP is related to the special trimer structure.