To address the issue of mechanical heterogeneity and structural failure in traditional anisotropic aerogels under complex stress fields, this study proposes a synergistic strategy combining bubble templating with freeze-casting. This approach enables the fabrication of an elastic carbon aerogel with three-dimensionally isotropic structural characteristics. Using aramid nanofibers as the matrix skeleton, the incorporation of graphene oxide reduces the surface tension of the solution while enhancing system viscosity, effectively suppressing bubble coalescence and ultimately yielding a carbon aerogel with a spherical cavity structure. The resulting aerogel exhibits nearly identical physical properties across all three spatial dimensions. Notably, it maintains exceptional structural stability (plastic deformation < 2.9%) even under 80% compressive strain and demonstrates ultra-wide temperature adaptability. This work provides a novel design strategy for high-performance porous materials.

High-performance thermal interface materials (TIMs) are highly sought after for modern electronics. Two-dimensional (2D) materials as vertical aligned fillers can optimize the out-plane thermal conductivity (k_⊥), but their excessively high content or intrinsic rigidness deteriorate TIMs softness, leading to worsening for thermal contact resistance (R_contact). In this study, 2D graphene materials are fabricated into lightweight and soft graphene foams (GFs) with high-orientation, acting as vertical filler frameworks to optimize the k_⊥ and R_contact for vertical GF (VGF) TIMs. The VGF-TIM has a high k_⊥ of 47.9 W·m⁻¹·K⁻¹ at a low graphene content of 15.5 wt.%. Due to the softness and low filler contents of GFs, the VGF-TIM exhibits a low compressive module (4.2 MPa), demonstrating excellent compressibility. The resulting TIM exhibit a low contact resistance of 24.4 K·mm²·W⁻¹, demonstrating 185.1% higher cooling efficiency in practical heat dissipating scenario compared to commercial advanced TIMs. This work provides guidelines for the design of advanced TIMs and their applications in thermal management.