Large, perfect Cs2Nb4O11 crystals were prepared by off-stoichiometric melt growth, and their electrical properties were studied. The crystals have a noncentrosymmetric orthorhombic structure (sp. gr Pnn2) at room temperature and undergo a phase transition at 164 degreesC, which is accompanied by a strong anomaly in c-axis dielectric permittivity and seems to be due to ferroelectric ordering. The crystals exhibit high ionic conductivity.