The present invention relates to a cesium borosilicate compound, a nonlinear optical crystal of cesium borosilicate, and a preparation method therefor and a use thereof. The cesium borosilicate compound has a chemical formula of Cs2B4SiO9 and a molecular weight of 481.15, and is prepared using a solid phase method. The nonlinear optical crystal of the cesium borosilicate compound has a chemical formula of Cs2B4SiO9 and a molecular weight of 481.15, does not have a center of symmetry, belongs to the tetragonal system with space group I4 and unit-cell parameters a=6.731(3) Å, c=9.871(9) Å and V=447.2(5) Å3, and has a wide transmittance range. The shortest ultraviolet cutoff edge is smaller than 190 nm, the frequency doubling effect of the crystal is 4.6 KDP, and the crystal is grown by a high-temperature solution spontaneous crystallization method and a flux method. The crystal has advantages of high growth rate, being transparent and inclusion free, low cost having a wide transmittance range, high hardness, good mechanical property, being crack resistant and not prone to deliquescence, being easy to process and store, and the like. The crystal is widely applied to manufacturing of nonlinear optical devices such as frequency doubling generators, frequency up-converters, frequency down-converters or optical parametric oscillators.