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High-efficient heat dissipation materials are urgently required in advanced electronic packaging technology because effectively releasing the internal heat flow density of electronic devices is a key factor during their operation. In this work, a novel vertical graphene nanosheets/carbon fibers (VGNs/CF) composite film, with a vertically oriented structure and excellent heat dissipation properties, is fabricated on the stainless steel substrate by a facile thermochemical growth method. The preparation of composite film is green, safe, and highly efficient. CF is used as a thermally conductive filler to provide thermal conductivity channels for VGNs, and both of them construct a continuous thermally conductive network. The through-plane thermal conductivity of the VGNs/CF composite film could reach 17.7 W/(m·K), and the addition of CF significantly improved the heat dissipation performance of the composite film compared with the pure VGNs film (13.9 W/(m·K)). Conclusively, the simple preparation method and outstanding thermal conductivity capacity of the VGNs/CF composite film are expected to meet the application requirements of the electronics industry.