In order to achieve diversification of material functions, extend the service life of materials, and develop the excellent properties of materials themselves, this paper takes elastic polyurethane (EPU) as the matrix and thermoplastic polyurethane (TPU) as the transition phase, a series of shape memory EPU-TPU composites with self-healing function were prepared based on the different proportions of EPU and TPU. The structure, thermal properties, mechanical properties, and shape memory properties of the raw materials and composites were tested and characterized by nuclear magnetic resonance (NMR), Fourier transform infrared spectroscopy (FTIR), differential scanning calorimetry (DSC), and a universal testing machine. The self-healing performance and self-healing mechanism of composites were analyzed. The results show that the shape memory effect of EPU-TPU (3∶7) is the best, with a fixed rate of 100% and a recovery rate of 98.9%. It takes more than 258 s to recover from the temporary curled shape to the initial strip shape, with fast thermal response. In addition, EPU-TPU (3∶7) and EPU-TPU (2∶8) also show good self-healing ability, with the strain after healing reaching about 600%.