Biocompatible poly(4‐styrenesulfonic acid‐co‐maleic acid)‐stabilized GdF3 : Eu3+(Tb3+) nanoparticles were obtained by a one‐step coprecipitation method in ethylene glycol or water. The particles are very small (3 nm), have a narrow size distribution, and were detectable by fluorescence, magnetic resonance, and X‐ray contrast imaging. These properties allow multimodal imaging, which has prospective applications in the simultaneous and detailed detection of diseased tissues.