AbstractFillers play a decisive role in the mechanical properties of polymer composites. In this paper, different particle sizes of nitroguanidine were obtained to regulate the internal filler structure of triple‐base propellants (TBP) to improve their mechanical response in different environments. A series of morphological and structural characterizations on nitroguanidine (NQ) particles were conducted using techniques. The results indicated that the obtained NQ particles maintained a high level of crystalline quality while preserving their molecular integrity. The mechanical properties of TBP were systematically evaluated under various loading conditions, including cryogenic tensile, compressive, and impact loads, as well as dynamic thermomechanical effects. Additionally, three‐point bending simulations were employed to elucidate the mechanical responses and damage mechanisms. Under axial tensile and compressive loads, reducing the particle size of NQ significantly enhanced the tensile and compressive strength. The maximum tensile strength and compressive strength can reach 344.62 MPa and 104.79 MPa. Moreover, the compressive failure mode transitioned from cracking to axial shrinkage. Conversely, when subjected to radial bending loads, TBP exhibited contrasting behavior, including a decrease in the glass transition temperature from 84.73°C to 76.93°C and a non‐monotonic trend in impact strength (initially increasing from 4.96 to 8.85 kJ/m2 and then decreasing to 2.27 kJ/m2). This study provides valuable insights into the mechanical performance of TBP, supporting the development of high‐energy, high‐strength TBP formulations.Highlights SEM analysis confirms the pronounced orientation effect of rod‐like NQ. The orientation and particle size of NQ decide TBP's radial impact resistance. Submicron NQ enhances the compression resistance property of TBP. Submicron NQ brings about a shift in the microscopic damage morphology of TBP.
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