Hydroxyl terminated polybutadiene (HTPB) coating is widely used in a solid rocket motor, but an aging phenomenon exists during long-term storage, which causes irreversible damage to the performance of this HTPB coating. In order to study the effect of aging on the dynamic mechanical properties of the HTPB coating, the thermally-accelerated aging test was carried out. The variation of maximum elongation and crosslinking density with aging time was obtained, and a good linear relationship between maximum elongation and crosslinking density was found by correlation analysis. The changing regularity of dynamic mechanical properties with aging time was analyzed. It was found that with the increase of aging time, T g of HTPB coating increased, T α , tan β and tan α decreased, and the functional relationships between the loss factor parameters and crosslinking density were constructed. The storage modulus and loss modulus of HTPB coating increased with the increase of aging time, and decreased with the increase of pre-strain. The aging enhanced the Payne effect of HTPB coating, while the pre-strain had a weakening effect. In view of the Payne effect of HTPB coating, the crosslinking density was introduced into Kraus model as aging evaluation parameter, and the crosslinking density modified models with and without pre-strain were established. The proposed models can effectively solve the problem that the Kraus model has a poor fitting effect under the condition of small strain (generally less than 1%) and on the loss modulus, which have improved the correlations between the fitting results and the test results.Polymers 2020, 12, 403 2 of 20 of 1 H NMR (nuclear magnetic resonance), and analyzed the influence of the crosslinking density on the macro-mechanical properties.It was found that with the increase of crosslinking density, the hardness and modulus of the material increased linearly, while the elongation at break decreased linearly. Katarzyna et al. [5] found that the existence of crosslinking resulted in the increase of the glass transition temperature T g . Actually, the linear relationship equation between T g and crosslinking density was derived in the study of Fox and Loshaek [6]. Although the linear equation was not completely consistent with some later results [7-9], they also came to the same conclusion that the crosslinking can increase the glass transition temperature of the polymer. In the study of Celina et al. [10], it was found that the crosslinking density of HTPB elastomers increased with the aging time. The mainly aging reaction was oxidation crosslinking, and the change of crosslinking density affected the mechanical properties of the material. Byungwoo et al. [11] also got the same conclusion. The test results demonstrated that the crosslinking density increased with the increase of aging temperature and aging time, and the crosslinking changed with the change of aging condition. The functional relationship between strain energy density and crosslinking density was established.Dynamic mechanical ...