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These systems can concentrate a large payload of paramagnetic sites in the region where they localize, thus increasing the sensitivity of the technique. In addition, when attached to the silica surface, the Gd<jats:sup>III<\/jats:sup> complexes reduce their rotational tumbling motion, which leads to an improvement of their performance as relaxation agents. In this review, we describe different strategies to confine paramagnetic species into porous silica. The relationship between the structural and dynamic parameters of conjugated Gd complexes on the surface of the MSNs and their effectiveness as relaxation agents is discussed, examining how the magnetic properties of the probes are influenced by the characteristics of the nanoparticles. Special attention is addressed to clarify the effect of silica support, in terms of porosity and surface reactivity, on the relaxometric properties of the final solids. 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