The invention provides a cesium rubidium fluoroboroaluminate nonlinear optical crystal and its preparation method and application. The chemical formula of the crystal is CsRbAl 2 (B 3 o 6 ) 2 f 2 , the molecular weight of the crystal is 567.19, the structure of the crystal belongs to the hexagonal system, and the space group is P-62c , the cell parameters are a =b=6.9807Å, c =8.057Å, α = β =90°, gamma =120°, the unit cell volume is 340.02Å 3 . The crystals can be grown by a pulling method or a high-temperature solution method. The nonlinear optical performance of the crystal of the invention is close to KBBF, and can be used for stepwise frequency doubling of Nd:YAG (λ=1064 nm) lasers to generate harmonic light output shorter than 200 nm. In addition, the crystal of the present invention has a single crystal structure, is colorless and transparent, has good thermal stability, does not use highly toxic raw materials for synthesis, can grow in an air atmosphere, and has no obvious layered growth habit.