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[en] Highlights: • A macroscopic multifunctional graphene-based aerogel with three-dimensional interconnected networks was fabricated. • Nd2O3 nanoparticles were incorporated with graphene sheets to assemble macroscopic graphene monoliths under mild conditions. • The rGO/Nd2O3 aerogel showed remarkable adsorption capacity and recycling regeneration properties towards different types of dyes, especially for anionic dyes. - Abstract: We report a one-step facile fabrication of macroscopic multifunctional graphene-based aerogel with three-dimensional interconnected networks under the synergistic effects of the reduction of graphene oxide sheets by L-ascorbic acid and in situ simultaneous deposition of nanoparticles on graphene sheets. The functional components, Nd2O3 nanoparticles, can be easily incorporated with graphene sheets to assemble bulk macroscopic graphene materials under mild conditions. The reduced graphene oxide/neodymium oxide (rGO/Nd2O3) aerogel showed remarkable adsorption capacity towards different types of dyes, especially for anionic dyes, with the adsorption capacity for indigo disulphonate (ID) being more than 220 mg g−1 within one hour while the adsorption capacity at equilibrium is as high as 397 mg g−1. The method proposed is proven to be universal to induce macroscopic assembly of reduced graphene sheets with rare earth metal oxides and thus facilitates to accessing various graphene-based multifunctional nanocomposites in the form of macroscopic aerogels.