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Uniform Nd³⁺-doped LuVO₄ nanophosphors have been synthesized for the first time in literature by using a poliol-based method at 120 °C from Nd³⁺ and vanadate precursors. After optimizing the Nd doping level, these phosphors present intense luminescence in the near-infrared biological windows. The X-ray attenuation capacity of the optimum nanophosphor has been found to be higher than that of a commercial X-ray computed tomography contrast agent. After surface coating with polyacrylic acid, such nanoparticles present high colloidal stability in physiological pH medium and high cell viability. Because of these properties, the developed Nd³⁺-doped LuVO₄ nanoparticles have potential applications as a bimodal probe for NIR luminescent bioimaging and X-ray computed tomography.