High-k polymer nanocomposites have considerable potential in energy storage and dielectric applications because of their ease of processing, flexibility, and low cost. Core-shell nanoarchitecture strategies are versatile and powerful tools for the design and synthesis of advanced high-k polymer nanocomposites. Recent and in-progress state-of-the-art advancements in the application of core-shell nanoarchitecture strategies to design and prepare high-k polymer nanocomposites are summarized. Special focus is directed to emphasizing their advantages over conventional melt-mixing and solution-mixing methods: first, homogeneous nanoparticle dispersion can be easily achieved even in highly loaded nanocomposites; second, the dielectric constant of the nanocomposites can be effectively enhanced and meanwhile the high breakdown strength can be well-preserved; third, for nanocomposites filled with electrically conductive nanoparticles, dielectric loss can be effectively surpressed, and meanwhile a high dielectric constant can be achieved. In addition, fundamental insights into the roles of the interfaces on the dielectric properties of the nanocomposites can be probed. The last part of the article is concluded with current problems and future perspectives of utilizing the core-shell nanoarchitecture strategies for the development of high-k polymer nanocomposites.