Balancing the wide band gap, large second harmonic generation (SHG) response, and moderate birefringence are significant but addressable challenges for designing nonlinear optical (NLO) materials. Based on the band-gap engineering in perovskite solar cell materials, we have successfully synthesized a new fluorotellurite, BaF2TeF2(OH)(2) , which exhibits a pseudo-Aurivillius structure and crystallizes in a noncentrosymmetric and polar space group Pmn2(1). The physical property measurements show that this material can effectively balance the requirements among the short UV absorption edge (similar to 205 nm), large SHG response (similar to 3 X KDP) and moderate birefringence similar to 0.078@350-700 nm) and is a promising ultraviolet NLO crystal.