Rational design of 2D materials is crucial for the realization of their profound implications in energy and environmental fields. The past decade has witnessed significant developments in 2D material research, yet a number of critical challenges remain for real‐world applications. Nanoscale assembly, precise control over the orientational and positional ordering, and complex interfaces among 2D layers are essential for the continued progress of 2D materials, especially for energy storage and conversion and environmental remediation. Herein, recent progress, the status, future prospects, and challenges associated with nanoscopic assembly of 2D materials are highlighted, specifically targeting energy and environmental applications. Geometric dimensional diversity of 2D material assembly is focused on, based on novel assembly mechanisms, including 1D fibers from the colloidal liquid crystalline phase, 2D films by interfacial tension (Marangoni effect), and 3D nanoarchitecture assembly by electrochemical processes. Relevant critical advantages of 2D material assembly are highlighted for application fields, including secondary batteries, supercapacitors, catalysts, gas sensors, desalination, and water decontamination.

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Graphene, despite being the best known strong and electrical/thermal conductive material, has found limited success in practical applications, mostly due to difficulties in the formation of desired large-scale highly organized structures. Our discovery of a liquid crystalline phase formation in graphene oxide dispersion has enabled a broad spectrum of highly aligned graphene-based structures, including films, fibers, membranes, and mesoscale structures. In this review, the current understanding of the structure-property relationship of graphene oxide liquid crystals (GOLCs) is overviewed. Various synthetic methods and parameters that can be optimized for GOLC phase formation are highlighted. Along with the results from different characterization methods for the identification of the GOLC phases, the typical characteristics of different types of GOLC phases introduced so far, including nematic, lamellar and chiral phases, are carefully discussed. Finally, various interesting applications of GOLCs are outlined together with the future prospects for their further developments.

Inspired by mussel adhesive polydopamine (PDA), effective reinforcement of graphene-based liquid crystalline fibers to attain high mechanical and electrical properties simultaneously is presented. The two-step defect engineering, relying on bioinspired surface polymerization and subsequent solution infiltration of PDA, addresses the intrinsic limitation of graphene fibers arising from the folding and wrinkling of graphene layers during the fiber-spinning process. For a clear understanding of the mechanism of PDA-induced defect engineering, interfacial adhesion between graphene oxide sheets is straightforwardly analyzed by the atomic force microscopy pull-off test. Subsequently, PDA could be converted into an N-doped graphitic layer within the fiber structure by a mild thermal treatment such that mechanically strong fibers could be obtained without sacrificing electrical conductivity. Bioinspired graphene-based fiber holds great promise for a wide range of applications, including flexible electronics, multifunctional textiles, and wearable sensors.