[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.