“…Graphene, as the most important new material in 21st century, has given rise to ever‐rising attentions due to its excellent mechanical and chemicophysics properties, which thus is omnipresently applied in fields, such as energy, [ 1,2 ] catalyst, [ 3 ] lubrication, [ 4 ] separation, [ 5 ] and communication. [ 6 ] More importantly, it initiates research upsurge of 2D materials around the world, including its derivatives, [ 7 ] graphdiyne, [ 8 ] phosphorene, [ 9 ] transition metal dichalcogenide, [ 10 ] perovskite, [ 11 ] and so on. However, from laboratory to practical applications, an acknowledged challenge lies across graphene‐based materials, that is, mono/few layer graphene nanosheets are difficult to rapidly, orderly and compactly assemble into macrostructures (film, monoliths, fiber, complicated shape, and gel) with excellent performances, which tremendously restricts further practical applications.…”