High dielectric constant ceramics fillers are widely used as fillers in polymer matrix to prepare high performance dielectric composites. Homogeneous filler distribution in these composites films is found to be quite difficult to achieve balance between high dielectric constant and high breakdown strength. Herein, multilayer structured composites films containing nickelous hydroxide (Ni(OH)₂) as fillers, with different multilayered structures were designed and prepared, including 2–5 layers structure with various filler distribution. The effects of multilayer structure on the dielectric performance are explored by keeping the overall filler content constant. Combined with computer simulation, it is suggested that the variation in filler distribution in these films can effectively redistribute electric field intensity. Meanwhile, the dielectric constant and breakdown strength of the overall composites can be adjusted by changing the volume ratio between high filler content layer and low filler content layer. It is noted that at least 1/3 of the overall film volume should be occupied by a high breakdown strength layer to keep rather high overall breakdown strength. Moreover, high dielectric constant layer should be the outer layers to achieve overall high dielectric constant. Among all the layered structures investigated, the maximum energy density of 6.03 J/cm³ is obtained for film with a 3-layer nonsequential arrangement structure, which is 68% higher than single layer film with identical composition. This study provides some reference value for the preparation of multilayered dielectric polymer composites films for energy storage applications.

高介电常数陶瓷填料被广泛用作聚合物基体中的填料，以制备高性能介电复合材料。发现在这些复合膜中均匀的填料分布很难在高介电常数和高击穿强度之间达到平衡。此处，包含氢氧化镍（Ni（OH）₂）的多层结构复合膜）作为填料，设计并制备了具有不同多层结构的填料，包括具有不同填料分布的2-5层结构。通过保持整体填料含量恒定，探索了多层结构对介电性能的影响。结合计算机模拟，建议这些膜中填料分布的变化可以有效地重新分布电场强度。同时，可以通过改变高填料含量层和低填料含量层之间的体积比来调节整个复合材料的介电常数和击穿强度。注意，高击穿强度层应占据总膜体积的至少1/3，以保持相当高的总击穿强度。此外，高介电常数层应该是外层，以实现整体高介电常数。在研究的所有分层结构中，最大能量密度为6.03 J / cm³是用于与3层的非顺序排列的结构，这是比用相同组合物的单层膜更高68％膜而得到。该研究为储能应用中多层介电聚合物复合薄膜的制备提供了参考。