Assembling titanium carbide (Ti ₃ C ₂ T _x ) MXene nanosheets into macroscopic films presents challenges, including voids, low orientation degree, and weak interfacial interactions, which reduce mechanical performance. We demonstrate an ultrastrong macroscopic MXene film using liquid metal (LM) and bacterial cellulose (BC) to sequentially bridge MXene nanosheets (an LBM film), achieving a tensile strength of 908.4 megapascals. A layer-by-layer approach using repeated cycles of blade coating improves the orientation degree to 0.935 in the LBM film, while a LM with good deformability reduces voids into porosity of 5.4%. The interfacial interactions are enhanced by the hydrogen bonding from BC and the coordination bonding with LM, which improves the stress-transfer efficiency. Sequential bridging provides an avenue for assembling other two-dimensional nanosheets into high-performance materials.

Despite recent progress in the synthesis and application of graphene-based aerogels, some challenges such as scalable and cost-effective production, and miniaturization still remain, which hinder the practical application of these materials. Here we report a large-scale electrospinning method to generate graphene-based aerogel microspheres (AMs), which show broadband, tunable and high-performance microwave absorption. Graphene/Fe₃O₄ AMs with a large number of openings with hierarchical connecting radial microchannels can be obtained via electrospinning-freeze drying followed by calcination. Importantly, for a given Fe₃O₄:graphene mass ratio, altering the shape of aerogel monoliths or powders into aerogel microspheres leads to unique electromagnetic wave properties. As expected, the reflection loss of graphene/Fe₃O₄ AMs-1:1 with only 5 wt.% absorber loading reaches −51.5 dB at 9.2 GHz with a thickness of 4.0 mm and a broad absorption bandwidth (R_L < −10 dB) of 6.5 GHz. Furthermore, switching to coaxial electrospinning enables the fabrication of SiO₂ coatings to construct graphene/Fe₃O₄@SiO₂ core‒shell AMs. The coatings influence the electromagnetic wave absorption of graphene/Fe₃O₄ AMs significantly. In view of these advantages, we believe that this processing technique may be extended to fabricate a wide range of unique graphene-based architectures for functional design and applications.