The fast-charging performance of conventional lithium-ion batteries (LIBs) is determined by the working temperature. LIBs may fail to work under harsh conditions, especially in the low-temperature range of the local environment or in the high-temperature circumstances resulting from the release of substantial Joule heating in the short term. Constructing a thermal engineering framework for thermal regulation and maintaining the battery running at an appropriate temperature range are feasible strategies for developing temperature-tolerant, fast-charging LIBs. In this work, we prepare phase change nanocapsules as a thermal regulating layer on the cell surface. The polyurea shells of the nanocapsules are decorated with polyaniline, where the molecular vibration of polyaniline is enhanced under solar irradiation, enabling light-to-heat conversion that achieves an effective temperature increment at low temperatures. Based on the large latent heat storage capability of the n-octadecane core in the nanocapsules, the thermal regulating layer is sufficient to modulate strong heat release when operating LIBs at a high current rate, which efficiently prevents strong side reactions at high temperatures or even the occurrence of thermal runaway. This work highlights the promise of optimizing the operating temperature with a thermal regulator to ensure the safety and performance stability of fast-charging LIBs.