“…[ 4 , 6 ] When applied practically, the nanosized graphene particles always need to be assembled together as certain format of macrostructures to support key structures and functions for various smart devices and systems, such as working electrodes of micro‐supercapacitors and sensing elements of flexible electronics. [ 7 , 8 ] In comparison with 1D (e.g., graphene‐based filaments, yarns, and composite fibers) [ 9 , 10 , 11 ] and 2D (e.g., graphene‐based thin films, papers, and fabrics) [ 12 , 13 ] geometries with small, thin, and/or binder/substrate‐supported natures, the graphene‐based 3D aerogels, [ 14 ] hydrogels, [ 15 ] foams, [ 16 ] millispheres, [ 17 ] and laminated structures/composites [ 18 , 19 ] were also intriguingly focused as another important macroscopic ensembles, exhibiting multiple unique characteristics including free‐standing and/or binder‐free structures, widely scaled and highly designable configurations, and organized networking architectures with interconnected nanoparticles/ domains. [ 20 ] Hence, the building of macroscopic 3D graphene has become a significant topic for satisfying the continuously upgraded structures and functions in various novel devices, such as artificial skins and muscles, wearable electronics, biomimetic surfaces, thin‐film batteries, and soft robots.…”