Graphene-like allotropes (e.g., nanotube, buckyball, and graphyne) lead to a 2D wonderland by realizing distinct material features by being atomically thin while also being mechanically robust constituents. They are chemically synthesized at the nanoscale and applied to small devices, while their large-scale applications require methods to design and realize their structures that will enable their synergistic function, which can be challenging. Natural lattice materials (e.g., diatom and bone structure, insect wings and silk structures) gain material advantages from their unique hierarchical structures, enabling them to assemble their basic building blocks at multiple length scales and reach multifunctionalities. Design principles learned from nature may lead to innovative lattice structures composed of graphene-like allotropes for achieving advanced material functions (e.g., mechanical strength, lightweight, thermal, optical, acoustic, and electronic features).

This Method Collection aims to gather methods in theoretical design and experimental synthesis of graphene and graphene-like architect materials, including but not limited to: multiscale computational modeling, high-throughput simulation, optimization with advanced artificial intelligence, chemical reactions, 3D printing, photolithography, liquid infiltration, lyophilization, and so on. Massive applications include semiconducting devices, energy storage, photosynthesis and energy harvest, active media for packaging and drug delivery, sound/light/thermal cloak, lightweight structural materials, separation membranes for liquid/gas filtration, and their combinations. Taking advantage of the size‐dependent properties typical of graphene-like allotropes in the forms of nanoparticles, nanowires, and nanofilms, these architect materials redefine the limits of accessible multi-dimensional design space of material functions throughout different disciplines.