In order to accurately describe the transverse relaxation characteristic and stress relaxation modulus of HTPB coating during pre-strain thermal aging process, a one month thermal aging test was carried out at 70 C with pre-strain of 0％, 3％, 6％ and 9％, respectively. The low-field 1H NMR and stress relaxation modulus tests were carried out for HTPB coating at different aging stages. The stress relaxation model considering the molecular chains was proposed according to the changes of crosslinking chain and dangling chain of HTPB coating during pre-strain aging. The results showed that with the increase of aging time, the decay rate of transverse relaxation curve became faster, the transverse relaxation time decreased, the value of combined parameter qMrl increased, the proportion of crosslinking chain decreased, while the proportion of dangling chain increased. Moreover, the stress relaxation modulus increased, the crosslinking network structure of HTPB coating became denser and the degree of cross-linking increased. At the initial aging stage, the pre-strain will destroy the crosslinking network structure of HTPB coating to a certain extent. With the increase of aging time, the effect of pre-strain will gradually weaken and the influence of aging on materials will gradually increase. The correlations between the stress relaxation model considering the molecular chains and the test results were more than 0.9950, which can accurately describe the stress relaxation modulus of HTPB coating during the pre-strain thermal aging process.