Abstract We prepared novel mesoporous organosilica nanoparticles with internal metal‐chelating diethylenetriametetraacetic acid groups (DTTA‐MSNPs) by co‐condensation and decorated them with fluorescent moieties. We studied the binding of transition metal ions such as copper(II), cobalt (II) and gadolinium (III) by DTTA‐MSNPs, and found high uptake of these metals. In particular, DTTA‐MSNPs uptake ~1.1×10 5 Gd 3+ per particle and possess a high r 1 relaxivity of 15.27 mM −1 s −1 . Thus, DTTA‐MSNPs may find applications in metal sequestration and in MR imaging and neutron capture therapy.