Single crystals of bismuth germanate Bi4(GeO4)3having the eulytine structure, space groupTd6, were grown. They were crucible‐free pulled from a pool of molten material produced in its own powder at 1040°C by a thermal imaging technique. The material has an index of refraction of 2.07 and transmits light between 0.4 and 6.0 &mgr;. The electro‐optic coefficientr41was determined to be 1.03·10−10cm/V. Although materials with higherr41values are known, Bi4(GeO4)3may find applications because the growth of large crystals appears possible by classical pulling techniques. A large variety of chemical substitutions are possible in the eulytine structure and might lead to improvements in the magnitude ofr41.