It is urgent for polyurethane (PU) damping materials to broaden the effective damping range. Based on the designability of PU, this study is focused on the role of long dangling chain, wherein prepared by the reaction of polyethylene glycol monomethyl ether with toluene-2,4-diisocyanate. Notably, the introduction of long dangling chain not only makes the dangling chain longer and enhances the intermolecular interaction but also equips the dangling chain with strong polar carbamate group, bringing about more excellent compatibility of the soft and hard segments and lower degree of microphase separation under the condition of hydrogen bonding. The results show that the damping performance increases with the synergistic effect of significant hydrogen bonding and decreased degree of microphase separation, and the effective damping temperature range (tan δ ≥ 0.3) can exceed 150°C (−50°C to 100°C). Simultaneously, the addition of long dangling chains endows PU with self-healing property, the self-healing rate of system reaches maximum 70% with shore A hardness of 15 because of the synergistic effect above with the addition of 60% dangling chain, which extends the service life of PU damping materials.