The present invention relates to a compound chlorine barium borate, a chlorine barium borate nonlinear optical crystal, and a preparation method and uses of the chlorine barium borate nonlinear optical crystal. According to the present invention, the chemical formula of the compound is Ba7B3O11Cl, the molecular weight is 1205.26, and the compound is synthesized by adopting a solid phase reaction method; the chemical formula of the chlorine barium borate nonlinear optical crystal is Ba7B3O11Cl, the molecular weight is 1205.26, the crystal does not have the symmetry center and belongs to the hexagonal crystal system, the space group is P6[3]mc, and the cell parameters are as the follows: a is 11.2266 (17) angstrom, c is 7.214 (2) angstrom, Z is 2, and V is 787.4 (3) angstrom; the frequency doubling effect of the crystal powder achieves the 0.5 time of the KDP (KH2PO4); and the crystal has characteristics of large mechanical hardness, easy cutting, easy polish processing and easy preservation, and is widely applied in preparation of frequency doubling generators, frequency up-convertors, frequency down-convertors, or optical parameter oscillators and other nonlinear optical devices.