Microspheres of lithium hydroxide (LiOH) were produced from in-flight solidification of droplets formed by the disintegration of an acoustically driven, mechanically vibrated cylindrical liquid jet of molten LiOH. The molten material at 470 to 480°C was fed through a 25-gauge (0.0267-cm bore diameter) nozzle, interiorly electroplated with silver, under ∼27.6-kPa (4-psig) pressure, and at a mechanical vibration frequency of 10 Hz. The resulting jet issued into a 5.5-cm-diam vertical glass drop tube entraining a 94.5 cm3/s (12 ft3/h) argon gas stream at 75°C. The 100-cm-long drop tube was sufficient to allow the droplets of molten LiOH resulting from jet disintegration to solidify in-flight without catastrophic thermal shock, being then collected as solid microspheres. These LiOH microspheres were then vacuum processed to lithium oxide (Li2O). Preliminary experiments resulted in microspheres with diameters varying from 120 to 185 µim, but with evidence of impurity contamination occurring during the initial stages of the process.