Highly thermal conductive polymer-based materials are essential for modern microelectronic devices. However, conventional thermal conductive polymer-based composites exhibit constrained thermal conductivity even at a high content of highly thermal conductive fillers due to the lack of significant thermal conductive paths. In this work, effective thermal conductive paths were constructed with macro recycled graphene film fragments that were vertically arranged by a method of area restricting in the vertical direction under mechanical force. The resulting composites with vertically arranged structure displayed highly through-plane thermal conductivity of 20.97 W m⁻¹ K⁻¹ at 32.63 wt% graphene film fragments loading. Another three contrast experiments in different adding ways of fillers were as well accomplished to confirm the excellent vertically arranged structure. This study not only provides a simple way to obtain highly thermal conductive composites but also offers a strategy of making full use of wastes from industrial applications. The facile method for obtaining the superhigh though-plane thermal conductivity enlightens us to practical application. The recycled graphene films as millimeter-particles in this study can be expanded to other millimeter-particles arrangements. The mechanical force used for vertically arranged structure can be broadened to other forces such as vacuum or hydraulic pressure.

高导热聚合物基材料对于现代微电子设备至关重要。然而，由于缺乏显着的导热路径，传统的基于导热聚合物的复合材料即使在高导热填料含量高的情况下也表现出受限制的导热率。在这项工作中，有效的导热路径是用宏观回收的石墨烯薄膜碎片构建的，这些碎片通过机械力在垂直方向上的面积限制方法垂直排列。所得的具有垂直排列结构的复合材料显示出 20.97 W m ^-1  K ^{-1 的}高贯穿平面热导率在 32.63 wt% 的石墨烯薄膜碎片负载下。还完成了另外三个不同填料添加方式的对比实验，证实了优异的垂直排列结构。这项研究不仅提供了一种获得高导热复合材料的简单方法，而且还提供了一种充分利用工业应用废物的策略。获得超高穿透平面热导率的简便方法启发了我们的实际应用。本研究中回收的石墨烯薄膜作为毫米粒子可以扩展到其他毫米粒子排列。用于垂直排列结构的机械力可以扩展到其他力，例如真空或液压。