Polymer dielectrics play an irreplaceable role in electronic power systems because of their high power density and fast charge-discharge capability, but it is limited by their low stability in the temperature range of 25-200 °C. Rather than the introduction of one-dimensional fillers in polymers, we used a kind of multidimensional synergistic design to prepare Al2O3-TiO2-Al2O3/PI composites with layered structures by introducing multi-dimensional materials in polyimide (PI). In fact, the composite achieves much higher temperature stability than the pure PI film. The optimally proportioned composite has an energy density of 3.41 J cm-3 (vs. 1.48 J cm-3 for pure PI) even at 200 °C. Additionally, it reaches an impressive energy density retention of up to 90% and maintains an energy efficiency as high as 86% at 400 MV m-1 in the temperature range of 25-200 °C. The multidimensional coordination design is proposed to obtain composite films, and provides a feasible strategy in the study of polymer-based composites with high-temperature performance.