The removal and separation of uranium from aqueous solutions are quite important for resource reclamation and environmental protection. Being one of the most effective techniques for metal separation, adsorption of uranium by a variety of adsorbent materials has been a subject of study with high interest in recent years. However, current methods for monitoring the adsorption process require complicated procedures and tedious measurements, which hinders the development of processes for efficient separation of uranium. In this work, we prepared a type of luminescent mesoporous silica-carbon dots composite material that has high efficiency for the adsorption of uranium and allows simultaneous in situ monitoring of the adsorption process. Carbon dots (CDs) were prepared in situ and introduced onto amino-functionalized ordered mesoporous silica (SBA-NH2) by a facile microplasma-assisted method. The prepared CDs/SBA-NH2 nanocomposites preserved the high specific surface area of the mesoporous silica, as well as the fluorescent properties of the CDs. Compared with bare SBA-NH2, the CDs/SBA-NH2 nanocomposites showed much improved adsorption ability and excellent selectivity for uranyl ions. Moreover, the fluorescence intensity of the composites decreased along with the increase of uranium uptake, indicating that the CDs/SBA-NH2 nanocomposites could be used for on-site monitoring of the adsorption behavior. More interestingly, the adsorption selectivity of the composites for metal ions was in good agreement with the selective fluorescence response of the original CDs, which means that the adsorption selectivity of CDs-based composite materials can be predicted by evaluating the fluorescence selectivity of the CDs for metal ions. As the first study of CDs-based nanocomposites for the adsorption of actinide elements, this work opens a new avenue for the in situ monitoring of adsorption behavior of CDs-based nanocomposites while extending their application areas.