Research on phase change materials (PCMs) is booming in the context of global energy structure transitions and the challenge of dealing with temperature fluctuations in engineering materials. Polyurethane solid–solid phase change materials (PUSSPCMs) show great potential for thermal energy storage and temperature regulation because of their designable molecular structure, no risk of leakage, and high bulk stability. In this paper, the recent research progress on PUSSPCMs is systematically reviewed. Starting from the material system, the core preparation process of the PUSSPCMs was elucidated. At the performance improvement level, related performance studies on PUSSPCMs are systematically summarized, focusing on the introduction of dynamic covalent bonds and a nanofiller composite strategy to enhance the thermophysical properties of the materials. At the application level, innovative studies and thermomodulation advantages of PUSSPCMs in different fields are summarized. Finally, for green development, multifunctionalization, and bottlenecks in the scale-up preparation of PUSSPCMs, future research directions for balancing the performance requirements, conducting multi-scale simulations, and exploring green materials are proposed to provide theoretical references for the development and application of high-performance PUSSPCMs.