Core–shell upconversion [email protected]–organic framework ([email protected]) nanostructures are constructed by coating hexagonal NaYF4:Yb,Er nanoparticle (NP) cores with amino-functionalized iron carboxylate MOF shells. These nanostructures combine the near-infrared optical property of the UCNP cores and the T2-magnetic response (MR) imaging property of the MOF shells. After surface modification, the core–shell nanostructures are demonstrated as high-resolution nanoprobes for targeted luminescence/MR imaging both in vitro and in vivo. As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.