To enhance the sustainability of nuclear energy and protect the environment, the efficient extraction of uranium from various water sources has emerged as an essential strategy for addressing the long-term challenges of nuclear waste management. In this study, we designed phosphoryl-functionalized graphene (PG) for efficient uranyl adsorption and synthesized the material from fluorinated graphene using phosphoryl ethanolamine under solvothermal conditions. The resultant PG features a unique 2D structure equipped with solvent-exposed phosphoryl groups, making it highly suitable for uranium adsorption in aqueous solutions. Notably, PG demonstrated a high sorption efficiency (∼77%) with rapid extraction capability (∼5 min) for U(VI) from aqueous media at pH 7, achieving an adsorption capacity of 316 mg U g