Polymer nanocomposites combine the merits of polymer matrices and the unusual effects of nanoscale reinforcements and have been recognized as important members of the material family. Being a fundamental material property, thermal conductivity directly affects the molding and processing of materials as well as the design and performance of devices and systems. Polymer nanocomposites have been used in numerous industrial fields; thus, high demands are placed on the thermal conductivity feature of polymer nanocomposites. In this Perspective, we first provide roadmaps for the development of polymer nanocomposites with isotropic, in-plane, and through-plane high thermal conductivities, demonstrating the great effect of nanoscale reinforcements on thermal conductivity enhancement of polymer nanocomposites. Then the significance of the thermal conductivity of polymer nanocomposites in different application fields, including wearable electronics, thermal interface materials, battery thermal management, dielectric capacitors, electrical equipment, solar thermal energy storage, biomedical applications, carbon dioxide capture, and radiative cooling, are highlighted. In future research, we should continue to focus on methods that can further improve the thermal conductivity of polymer nanocomposites. On the other hand, we should pay more attention to the synergistic improvement of the thermal conductivity and other properties of polymer nanocomposites. Emerging polymer nanocomposites with high thermal conductivity should be based on application-oriented research.