The inherently formed liquid crystals (LCs) of graphene oxide (GO) in aqueous dispersions severely restrict the fabrication of large-size and structure-intact graphene aerogel bulk by an industry-applicable method. Herein, by developing a surfactant-foaming sol−gel method to effectively disrupt and reconstruct the inherent GO LCs via microbubbles as templates, we achieve the large-size and structure-intact graphene hydrogel bulk (GHB). After simple freezing and air-drying, the resulting graphene aerogel bulk (GAB) with a structure-intact size of about 1 m 2 exhibits a superelasticity of up to 99% compressive strain, ultralow density of 2.8 mg cm −3 , and quick solar-thermal conversion ability. The modified GAB (GABTP) shows a high decomposition temperature (T max ) of 735 °C in air and a low heat storage capacity. These excellent performances make the GABs suitable for many practical applications, as proven in this work, including as high compressive force absorbers, high absorption materials for oils or dangerous solvents, superior solar-thermal management materials for rapid heater or controlled shelter, and high-efficiency fire-resistant and thermal insulation materials. The whole preparation process is easily scalable and cost-effective for mass production of structureintact multifunctional graphene aerogel bulk toward practical applications.

Microdevice integrating energy storage with wireless charging could create opportunities for electronics design, such as moveable charging. Herein, we report seamlessly integrated wireless charging micro-supercapacitors by taking advantage of a designed highly consistent material system that both wireless coils and electrodes are of the graphite paper. The transferring power efficiency of the wireless charging is 52.8%. Benefitting from unique circuit structure, the intact device displays low resistance and excellent voltage tolerability with a capacitance of 454.1 mF cm−2, superior to state-of-the-art conventional planar micro-supercapacitors. Besides, a record high energy density of 463.1 μWh cm−2 exceeds the existing metal ion hybrid micro-supercapacitors and even commercial thin film battery (350 μWh cm−2). After charging for 6 min, the integrated device reaches up to a power output of 45.9 mW, which can drive an electrical toy car immediately. This work brings an insight for contactless micro-electronics and flexible micro-robotics.

Highly compressible graphene-based monoliths with excellent mechanical, electrical, and thermal properties hold great potential as multifunctional structural materials to realize the targets of energy-efficiency, comfort, and safety for buildings, vehicles, aircrafts, etc. Unfortunately, the ultralow mechanical strength and limited macroscale have hampered their practical applications. Herein, ultrastrong superelastic graphene aerogel with infinite macroscale is obtained by a facile wet-press assembly strategy based on the novel superplastic air-dryable graphene hydrogel (SAGH). The SAGH with isotropic, open-cell, and highly porous microstructure is carefully designed by a dual-template sol-gel method. Countless SAGH "bricks" can be assembled together orderly by press to form the strongly combined wet-press assembled graphene aerogel (WAGA) "wall" after air-drying. The WAGA with highly oriented, dense, multiple-arch microstructure possesses arbitrary macroscale, outstanding compressive strength (47 MPa, over 10 times higher than the best ever reported), super elasticity (>97% strain), and high conductivity (378 S m −1 ). The strong adhesion is attributed to the tightly face-to-face contacted graphene interfaces caused by wet-press and air-drying. The WAGAs prove to be excellent multifunctional structural materials in the fields of high pressure/strain sensor, tunable mechanical energy absorber, high-performance fire-resistance, and thermal insulation. This facile strategy is easily extended to fabricate other similar metamaterials.

Graphene aerogels (GAs) with attractive properties have shown tremendous potentials in energy- and environment-related applications. Unfortunately, current assembly methods for GAs such as sol–gel and freeze-casting processes must be conducted in enclosed spaces with unconventional conditions, thus being literally inoperative for in situ and continuous productions. Herein, a direct slurry-casting method at open ambient conditions is established to arbitrarily prepare three-dimensional (3D) porous graphene oxide (GO) bulks without macroscopic dimension limits on a wide range of solid surfaces by retarding Ostwald ripening of 3D liquid GO foams when being dried in air. A subsequent fast thermal reduction (FTR) of GO foams leads to the formation of graphene aerogels (denoted as FTR-GAs) with hierarchical closed-cellular graphene structures. The FTR-GAs show outstanding high-temperature thermal insulation (70% decrease for 400 °C), as well as superelasticity (>1000 compression–recovery cycles at 50% strain), ultralow density (10–28 mg cm–3), large specific surface area (BET, 206.8 m2 g–1), and high conductivity (ca. 100 S m–1). This work provides a viable method to achieve in situ preparations of high-performance GAs as multifunctional structural materials in aircrafts, high-speed trains, or even buildings for the targets of energy efficiency, comfort, and safety.

The constructing of 3D materials with optimal performance is urgently needed to meet the growing demand of advanced materials in the high‐tech sector. A distinctive 3D graphene (3DG) is designed based on a repeated rebirth strategy to obtain a better body and performance after each round of rebirth, as if it is Phoenix Nirvana. The properties of reborn graphene, namely 3DG after Nirvana (NvG), has been dramatically upgraded compared to 3DG, including high density (3.36 times) together with high porosity, as well as better electrical conductivity (1.41 times), mechanical strength (32.4 times), and ultrafast infiltration behavior. These advantages of NvG make it a strong intrinsic motivation for application in capacitive deionization (CDI). Using NvG directly as the CDI electrode, it has an extremely high volumetric capacity of 220 F cm−3 at 1 A cm−3 and a maximum salt absorption capacity of 8.02~9.2 mg cm−3 (8.9–10.2 times), while the power consumption for adsorption of the same mass of salt is less than a quarter of 3DG. The “Phoenix Nirvana”‐like strategy of manufacturing 3D structures will undoubtedly become the new engine to kick‐start the development of innovative carbon materials through an overall performance upgrade.