Core/shell upconverting nanoparticles (UCNPs) of NaGdF4:Er3+, Yb3+/NaGdF4 (see figure) are shown to serve as a multimodal imaging probe that works for both background-free optical imaging and magnetic resonance imaging (MRI). The nonblinking and nonbleaching properties of UCNPs can contribute to minimization of possible artifacts in long-term imaging experiments. Owing to Gd3+ ions in the host matrix, contrast is enhanced in T-1-weighted MRI.