Abstracts: The mechanical strength was influenced by the quality of the crystal and interfacial interaction between energetic particles and polymeric binders. In this work, rod-like and hairy-spherical 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105) with a high crystal quality was modified by polydopamine (PDA) and hyperbranched polymers (HBP) grafting. The morphology of modified LLM-105 changed into a rough surface, resulting in the obvious enhancement of surface energies and adhesion work with the fluoropolymer. Further, the thermal behavior was slightly affected after surface modification due to the decomposition latent of PDA and HBP. Owing to the combined e chemical bonding of PDA and interlocking interaction of HBP, the creep resistance and mechanical strength of the modified LLM-105-based polymer bonded explosives (PBXs) were significantly improved, assisted by quantitative analysis of the interfacial strength. This strategy may provide insights to other composites requiring high mechanical performance.