Tailoring the Damping Thermal Response of Polyurethanes via Tunable Cross‐Linked Network Architectures

In response to the escalating demands for vibration attenuation within modern infrastructure, developing damping materials with high environmental adaptability is of paramount importance. However, traditional damping materials such as rubber are typically restricted by narrow effective windows (below 40°C). This study presents a synergistic strategy integrating molecular architecture design with stoichiometric regulation to develop crosslinked polyurethane systems featuring “programmable glass‐transition temperature ( T g )” By precisely modulating the molecular weight and concentration of crosslinkers, the microphase separation morphology is driven to evolve from a “sea‐island” to an “island‐sea” structure, enabling systematic tuning of the T g across a broad span from −32.38°C to 87.59°C. While each individual formulation sustains an effective damping (tan δ ≥ 0.3) window of approximately 40°C, the proposed design framework enables the precise positioning of these operational windows across a wide thermal spectrum from −45.65°C to 107.65°C. Furthermore, a T g prediction model ( R 2 = 0.99) was established, providing quantitative guidance for tailoring formulations to specific extreme environments. This work presents simple and feasible insights for the customized design of the effective damping temperature range of damping materials, which can provide guidance for the development of cross‐linked damping materials.