Two new metal borate-phosphates, Pb4O(BO3)(PO 4) (1) and Bi4O3(BO3)(PO 4) (2), have been successfully designed and synthesized. The structures of the title compounds were determined by single-crystal X-ray diffraction. The title compounds have similar crystal structures consisting of oxygen-centered (OPb4) or (OBi4) tetrahedra as well as isolated BO3 and PO4 groups. Structural comparison and the Madelung energy calculation indicate that the title compounds also exhibit a strong correlation with the known metal borates and phosphates. In addition, a strategy of BO3-PO4 substitution is proposed for designing new borate-phosphates. Thermal analyses, IR spectroscopy and UV-vis-NIR diffuse reflectance spectroscopy have also been performed