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Polymeric coating materials (PCMs) are promising candidates for developing next-generation flexible displays. However, PCMs are frequently subjected to external stimuli, making them highly susceptible to repeated damage. Therefore, in this study, a highly self-healing PCM based on a charge transfer complex (CTC) was developed, and its thermal, self-healing, and mechanical properties were examined. The self-healing material demonstrated improved thermal stability, fast self-healing kinetics (1 min), and a high self-healing efficiency (98.1%) via CTC-induced multiple interactions between the polymeric chains. In addition, it eliminated the trade-off between the mechanical strength and self-healing capability that is experienced by typical self-healing materials. The developed PCM achieved excellent self-healing and superior bulk (in-plane) and surface (out-of-plane) mechanical strengths compared to those of conventional engineering plastics such as polyether ether ketone (PEEK), polysulfone (PSU), and polyethersulfone (PES). These remarkable properties are attributed to the unique intermolecular structure resulting from strong CTC interactions. A mechanism for the improved self-healing and mechanical properties was also proposed by comparing the CTC-based self-healing PCMs with a non-CTC-based PCM.