▎ 摘　　要

Thermally conductive functionalized multilayer graphene sheets (fMGs) are efficiently aligned in large-scale,by,a vacuum filtration method at room temperature, as evidenced by SEM images and polarized Raman spectroscopy, A remarkably strong anisotropy in properties of aligned fMGs is observed. High electrical (similar to 386 S cm(-1)) and thermal conductivity (similar to 112 W m(-1) K-1 at 25 degrees C) and ultralow coefficient of thermal expansion (similar to-0.71 ppm K-1) In the in-plane direction of A-fMGs. are obtained Without any reduction process. Aligned fMGs are vertically assembled between contacted silicon/silicon surfaces with pure indium as a metallic medium. Thus-constructed three-dimensional-vertically aligned fMG thermal interfacial material (VA-fMG TIM) architecture has significantly higher equivalent thermal conductivity (75.5 W m(-1) K-1) and lower contact thermal resistance (5.1 mm(2) K W-1), compared with their counterpart from A-fMGs that are recumbent between silicon-surfaces.,This finding provides a throughout approach for a graphene-based TIM assembly as well as knowledge of vertically aligned graphene architectures, which may not only facilitate graphene's application in current demanding thermal management but also promote its widespread applications in electrodes of energy storage devices, conductive polymeric composites, etc.