In order to optimize the NMR assignment of 3, 4-dinitrofurazanfuroxan (DNTF), a combination of experimental NMR and computational GIAO-NMR techniques was utilized to distinguish the chemical shifts of ¹³C and ¹⁵N. One dimensional (1D) ¹³C and ¹⁵N NMR analyses were performed using DMSO-d₆, acetone-d₆ and CDCl₃ as solvent. All signals of DNTF were found in DMSO-d₆. In the ¹³C NMR, the chemical shifts were assigned by 2D INADEQUATE NMR experiment. Based on the geometry of DNTF optimized at the DFT-B3LYP/6-311+G(2d, p) level by using Guassian 09 program, the ¹³C and ¹⁵N NMR chemical shifts were calculated by GIAO method at different level, which agree with experimental data. Results show that the electro-withdrawing effect of the O(22) in furoxan cycle leads to large ¹³C chemical shift changes of C(9) and C(13), and makes C(9) appear in higher field than C(13).