AbstractFine particles of dense, high‐purity, crystalline BaTiO3were produced by flame‐spray pyrolysis. A 0.5‐M (Ba:Ti = 1:1) solution of barium acetate, titanium lactate, and water was aerosolized using an ultrasonic generator, and the droplets were delivered into the core of an annular diffusion flame (H2/air) reactor. For all investigated temperatures [∼1,000–∼2,000°C adiabatic], the generated powders were chemically pure, crystalline (primarily tetragonal phase with hexagonal and cubic polymorphs), and unagglomerated. At a low‐flame temperature (∼1,000°C ad.), the particles produced were hollow and irregularly shaped. Particles produced at higher flame temperatures (>∼1,500°C ad.) were dense and homogeneous. Particles showed a transition from a nonspherical porous morphology to a spherical dense morphology with increasing temperature. By increasing residence time, the temperature at which particles became spherical and dense was reduced. Flame‐spray pyrolysis provides a useful method for forming dense particles of high melting point materials by aeros