The influence of crystallographic orientation and rotation rate on the crystalline quality of Czochralski grown BaLiF3 crystals have been studied by neutron diffraction techniques. Analysis of the mosaicity of crystals showed that growth in the <111> direction with a flat interface resulted in crystals with good optical and crystalline quality. However, growth in the <100> direction with flat interface produced a low degree of optical quality but still with good crystallinity.