Deep-ultraviolet(U V)nonlinear optical(NLO)crystals with excellent performances are of great importance in laser science and technology.However,to design and synthesize an ideal deep-UV NLO material with a balance between second harmonic generation(SHG)response and UV cut-off edge is still a huge challenge.Herein,a new oxy-borate BaYOBO3(BaYBO)was designed and synthesized by substituting Be2+with Y3+from Sr2Be2B2O7.The BaYBO features a stable three-dimensional framework and satisfies the property balance between a large SHG response(~2.6×KH2PO4(KDP))and a short UV cut-off edge(<190 nm)as a promising deep-UV NLO candidate.The study of structure-property relationship indicates that the large SHG response of BaYBO is mainly attributed to the coplanar arrangement and large number density of BO3 triangles.These results demonstrate that substituting Be2+with Y3+cations is also a feasible strategy for developing new deep-UV NLO crystals.