Two novel zinc borate halides named Zn2BO3X center dot H2O (X = Cl, Br) were discovered through hydrothermal techniques. Both compounds are isomorphic and feature the layered structure similar to that of KBBF, consisting of the infinite planar [Zn2BO3X center dot OH2] (X = Cl, Br) layers. Compared with the weak ionic bond between adjacent layers in KBBF, the strong interaction of hydrogen bonds between layers in Zn2BO3X center dot H2O (X = Cl, Br) effectively enhances the interlayer force, contributing to eliminating the layering growth tendency. Optical measurements on these two NLO crystals revealed that they have a broad wavelength transparency window and a moderate NLO coefficient. Moreover, the theoretical calculations revealed that the linear and NLO properties primarily depended on the [BO3] and [ZnO3Cl/Br] groups in both crystals.