Highly vertically thermally conductive silicon rubber (SiR) composites are widely used as thermal interface materials (TIMs) for chip cooling. Herein, inspired by water transport and transpiration of Moso bamboo-forests extensively existing in south China, and guided by filler self-assembly simulation, bamboo-forest-like heat conduction networks, with bamboo-stems-like vertically aligned polydopamine-coated carbon fibers (VA-PCFs), and bamboo-leaves-like horizontally layered Al₂O₃(HL-Al₂O₃), are rationally designed and constructed. VA-PCF/HL-Al₂O₃/SiR composites demonstrated enhanced heat conduction properties, and their through-plane thermal conductivity and thermal diffusivity reached 6.47 W (mK)^-1 and 3.98 mm² s^-1 at 12 vol% PCF and 4 vol% Al₂O₃ loadings, which are 32% and 38% higher than those of VA-PCF (12 vol%) /SiR composites, respectively. The heat conduction enhancement mechanisms of VA-PCF/HL-Al₂O₃ networks on their SiR composites are revealed by multiscale simulation: HL-Al₂O₃ bridges the separate VA-PCF heat flow channels, and transfers more heat to the matrix, thereby increasing the vertical heat flux in composites. Along with high volume resistivity, low compression modulus, and coefficient of thermal expansion, VA-PCF/HL-Al₂O₃/SiR composites demonstrate great application potential as TIMs, which is proven using multiphysics simulation. This work not only makes a meaningful attempt at simulation-driven biomimetic material structure design but also provides inspiration for the preparation of TIMs.

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