<p>Designing of materials for effective uranium removal remains an open challenge. In the present work, we present a one-step co-condensation synthesis of a phosphonate functionalized ordered mesoporous silica (OMS-P). This novel material was characterized by various physicochemical methods (HR-TEM, SEM, N<sub>2</sub>sorption, XPS, solid NMR, low-angle XRD, and FTIR) and its ability to remove U(VI) by adsorption from aqueous solutions was studied. The maximum adsorption capacity reached 345 mg/g in 10 minutes, the highest reported up to day for silicas at pH = 4 and almost four times higher than for the unfunctionalized silica. Even more interestingly, the coexistence of other cations, such as Eu(III), did not affect adsorption capacity and selectivity. The adsorption results were evaluated based on various theoretical models in order to conclude regarding the kinetics. Moreover, the main interactions responsible for the increased U(VI) removal efficiency and in general the role of surface chemistry were analyzed by spectroscopic characterizations of OMS-P before and after adsorption.</p>