A new nonlinear optical material, the first fluoride selenite nitrate PbCdF(SeO3)(NO3), was successfully synthesized by traditional solid state reactions. This compound crystallizes in the polar space group of Pca2(1), and its structure features a novel 2D layered structure consisting of 1D lead nitrate chains and 2D cadmium selenite layers. PbCdF(SeO3)(NO3) exhibits a phase-matchable SHG efficiency of about 2.6 times that of KDP and a wide band gap of 4.42 eV. Its laser damage threshold was measured to be 135.6 MVV/cm(2), which is comparative to that of the reported Li-7(TeO3)(3)F with a short ultraviolet cutoff edge. Theoretical calculation confirmed that the synergistic effects of all the four functional units make PbCdF(SeO3)(NO3) a remarkable SHG material.