21:T553,Flexible and highly thermally conductive materials with consistent thermal conductivity (λ) during large deformation are urgently required to address the heat accumulation in flexible electronics. In this study, spring-like thermal conduction pathways of silver nanowire (S-AgNW) fabricated by 3D printing are compounded with polydimethylsiloxane (PDMS) to prepare S-AgNW/PDMS composites with excellent and consistent λ during deformation. The S-AgNW/PDMS composites exhibit a λ of 7.63 W m^-1 K^-1 at an AgNW amount of 20 vol%, which is ≈42 times that of PDMS (0.18 W m^-1 K^-1) and higher than that of AgNW/PDMS composites with the same amount and random dispersion of AgNW (R-AgNW/PDMS) (5.37 W m^-1 K^-1). Variations in the λ of 20 vol% S-AgNW/PDMS composites are less than 2% under a deformation of 200% elongation, 50% compression, or 180° bending, which benefits from the large deformation characteristics of S-AgNW. The heat-transfer coefficient (0.29 W cm^-2 K^-1) of 20 vol% S-AgNW/PDMS composites is ≈1.3 times that of the 20 vol% R-AgNW/PDMS composites, which reduces the temperature of a full-stressed central processing unit by 6.8 °C compared to that using the 20 vol% R-AgNW/PDMS composites as a thermally conductive material in the central processing unit.22:T4fe,Abstract Heterostructure fillers are crucial for enhancing the electromagnetic interference (EMI) shielding performance of composites, and the core lies in the regulation of their morphology. Inspired by the radial structures on marimo surfaces during growth, we propose a bioinspired heterostructure assembly strategy to fabricate novel marimo‐like hollow spherical reduced graphene oxide (hs‐rGO)@nickel‐catalyzed nitrogen‐doped carbon nanotubes (Ni‐NCNTs) and their corresponding polyimide aerogels. Benefiting from the synergistic design of multilevel porous architectures formed by the hollow microspheres in combination with the aerogel matrix, as well as radially aligned Ni‐NCNTs epitaxially grown on hs‐rGO surfaces, the resulting aerogels exhibit exceptional EMI shielding effectiveness, reaching up to 68 dB. Finite element simulations further elucidate the shielding mechanisms. Additionally, these aerogels exhibit rapid, durable pressure‐sensing performance due to their excellent resilience and conductivity. The multifunctional combination of high‐efficiency EMI shielding and mechanical sensing highlights their promising potential in next‐generation intelligent electronics, aerospace systems, and advanced communication technologies. image

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