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Uranium (Ⅵ) exists as many species in natural water systems. In the recent years, its contamination to groundwater has been reported more frequently. To investigate the effects of speciation on the removal of uranium, this work investigated the uranium adsorption behaviors of a polyamine-grafted silica composite named SAER at the concentration level of μg/L in the alkaline carbonate solutions with other four resins. Results suggested that the change of uranium speciation had minor effect on the adsorption efficiencies of SAER, except the addition of calcium. This was resulted from that the protonated tetraethylenepentamine had a much higher affinity to the electronegative uranyl-carbonate species, leading to the complete removal of uranium through the simultaneous anion exchange and chemical transformation mechanisms; Column experiments confirmed that merely a small portion of calcium while no magnesium cations were involved in the uranium adsorption in the simulated groundwater. Finally, the integrated removal mechanisms were proposed. Overall, this work demonstrated the feasibility of a novel adsorbent for the effective removal of uranium from different water matrices as well as the mechanisms underlying the interaction of uranium and the functional groups on the adsorbents. Furthermore, it enhanced the understanding of uranium removal under environmentally relevant conditions.