Graphene/graphene nanoribbons hybrid aerogel (GA/GNRs) was prepared via a hydrothermal process by using graphene oxide as precursor, and the graphene oxide nanoribbons unzipped from multi-walled carbon nanotubes were compound together. Various techniques were used to investigate the morphology, surface properties and structure of aerogel samples. Besides, the adsorption properties of the hybrid aerogel for the removal of U(VI) were further studied. The results showed that GNRs was grafted on the surface of graphene, and the specific surface area and porous pores structure were enhanced. The adsorption process of hybrid aerogel for U(VI) was pH-dependent, rapid, spontaneous and endothermic, and the maximum adsorption capacity for U(VI) was calculated to be 327.8 mg/g, which is expected to separate uranium from wastewater.