The LiSr3Be3B3O9F4 (LSBBF) single crystal with dimensions of 30 × 20 × 15 mm3 was grown from a LiF-NaBF4-B2O3-SrF2 flux system using a top-seeded solution growth method with a seed perpendicular to the (011) plane. The X-ray rocking curve, transmission spectra, refractive indices and laser-induced damage threshold have also been studied. The Sellmeier equations were derived from the measured refractive indices for the first time. According to the Sellmeier equations, the limits of type-I and type-II phase-matching (PM) frequency doubling wavelengths are 241 and 318 nm, respectively. It indicates that LSBBF is a potential UV nonlinear optical crystal for the fourth harmonic generation of Nd:YAG laser at 266 nm.