Interfacial interactions of polymers with 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105) directly influence the surface boating effects of LLM-105. The analyses of interactional models and strength at the atomic and molecular level will help to reveal the micro-mechanism of the interfacial interactions. In this work, molecular dynamics (MD) method was used to simulate the interfacial interactions of fluoropolymers (F₂₃₁₁, F₂₃₁₃, F₂₃₁₄, F₂₄₆₂) and polyurethane (Estane 5703) with LLM-105 at different crystal faces. Interactional mode and strength between the polymers and LLM-105 at different crystal faces were analyzed, and the screening principle of the polymer binders was preliminarily proposed. According to the principle, nitrifying bacterial cellulose (NBC, a new polymer) was selected and the interactions between NBC and LLM-105 were simulated. The effect of six polymers on the mechanical properties of LLM-105 was discussed using static elastic constant analysis. The simulation results show that the bonding energies of all polymers with LLM-105 at various crystal faces are positive and the increasing order of bonding strength is LLM-105/NBC≈LLM-105/Estane 5703>LLM-105/F₂₃₁₃≈LLM-105/F₂₃₁₄≈LLM-105/F₂₃₁₁>LLM-105/F₂₄₆₂. The (1 0 1) crystal face with the largest binding energy has the smallest exposed surface in the crystal(0.39%), while the(0 2 0) and (0 1 1) crystal faces with smaller binding energies have the larger exposed surface (>60% in total). The Van der Waals force is dominant in the interfacial interactions and is much higher than the electrostatic interactions. The polymers possessing strong interactions with LLM-105 simultaneously have good hydrogen-bonding donors and acceptors. The effective isotropic modulus and the Cauchy pressure values show that NBC, Estane 5703, and F₂₄₆₂ can slightly improve, F₂₃₁₁ and F₂₃₁₃ has no influence, and F₂₃₁₄ reduce the mechanical properties of LLM-105.