Abstract Overcoming the persistent trade‐off among thermal conductivity, mechanical compliance, and dynamic stability in elastic thermal interface materials (TIMs) remains a critical challenge. Conventional random‐filler approaches suffer from inefficient heat conduction, while pre‐formed thermal networks lack conformability adapt to dynamic interfaces a biomimetic solution involving dandelion‐inspired is presented, radially oriented graphene microspheres encapsulating gallium‐indium liquid metal nanoparticles (LMGS). This multi‐tiered design, which incorporates both the radial microscale structural architecture of the microspheres and their macroscopic stacking configuration, engenders microscale thermal conduction units that autonomously organize into a highly efficient 3D thermal network (11.1 W m −1 K −1 per vol%). Crucially, the graphene skeleton supports and confines the liquid metal, suppressing coalescence and leakage under stress. This innovative approach effectively addresses the challenges associated with filler dispersion and network infiltration. The radial architecture facilitates isotropic heat dissipation, while the inherent compliance of the microspheres combines with the polymer matrix to achieve a low compressive modulus and 94.7% rebound (40% compressing strain at 100 cycles). Consequently, LMGS‐based TIMs maintain vibration‐resistant conformal contact and excellent thermal stability under dynamic mechanical stresses. This bioinspired architectural paradigm decouples thermal and mechanical properties, offering a promising pathway for advanced thermal management in next‐generation flexible electronics and aerospace systems.
He et al. (Mon,) studied this question.