Uniform, hydrophilic 50 nm diameter Nd3+-doped Ba0.3Lu0.7F2.7 nanospheres are synthesized at 120 °C using a singular one-pot method based on the use of ethylene glycol as solvent, in the absence of any additive. The composition and crystal structure of the undoped material are analyzed in detail using ICP and XRD, which reveals a BaF2 cubic crystal structure that is able to incorporate 70 mol% of Lu ions. This finding contrasts with the reported phase diagram of the system, where the maximum solubility is around 30 mol% Lu. XRD proves as well that the Ba0.3Lu0.7F2.7 structure is able to incorporate Nd3+ ions up to, at least 10 mol%, without altering the uniform particles morphology. The Nd-doped particles exhibit near-infrared luminescence when excited at 810 nm. The maximum emission intensity with the minimum concentration quenching effect is obtained at 1.5% Nd doping level. X-ray computed tomography experiments are carried out on powder samples of the latter composition. The sample significantly absorbs X-ray photons, thus demonstrating that the Nd3+-doped Ba0.3Lu0.7F2.7 nanospheres are good candidates as contrast agents in computed tomography.