Vertical graphene nanowalls (VGNs) with excellent heat-transfer properties are promising to be applied in the thermal management of electronic devices. However, high growth temperature makes VGNs unable to be directly prepared on semiconductors and polymers, which limits the practical application of VGNs. In this work, the near room-temperature growth of VGNs was realized by utilizing the hot filament chemical vapor deposition method. Catalytic tantalum (Ta) filaments promote the decomposition of acetylene at ∼1600 °C. Density functional theory calculations proved that C2H* was the main active carbon cluster during VGN growth. The restricted diffusion of C2H* clusters induced the vertical growth of graphene nanoflakes on various substrates below 150 °C. The direct growth of VGNs successfully realized the excellent interfacial contact, and the thermal contact resistance could reach 3.39 × 10-9 m2·K·W-1. The temperature of electronic chips had a 6.7 °C reduction by utilizing directly prepared VGNs instead of thermal conductive tape as thermal-interface materials, indicating the great potential of VGNs to be directly prepared on electronic devices for thermal management.
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