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The development of safe and facile strategy processing novel high-energy nitrocellulose (NC)-based propellants is urgently needed but challenging recently. The energy additives commonly used at this stage are effective in improving the performance of nitrocellulose, but have the disadvantage of low density or high sensitivity. In the present work, 3-methyl-4-nitro-furoxan with N–O dipoles is exploited for the fabrication of nitrocellulose-based composites with good processability and enhanced mechanical properties by means of twin-screw extrusion technology. Their apparent viscosity is reduced to 93 kpas, which is 1.68 times lower than nitrocellulose and comparable to NC-NG (40wt%) composite. The tensile strain of NC-NMFO composites ranges from 3% to 12% and the impact strength is located between 28 kJ/m2 and 55 kJ/m2, which is significantly better than those of nitrocellulose with tensile strain of 2% and impact strength of 26 kJ/m2. This work could provide a promising alternative to process novel high-energy nitrocellulose (NC)-based propellants.