A two-dimensional (2D) nonlinear-optical (NLO) material could generate a breakthrough in the development of a nanoscale laser, especially in the range of high-energy and short-wavelength deep ultraviolet (DUV; <200 nm). KBe2BO3F2 (KBBF) is the only bulk crystal actually used in the DUV region. In this letter, we designed the new 2D KBBF family monolayer Al3LiB2O6F4 (2D-ALBF), which was predicted to have a broad DUV-vis transparent range and an enhanced NLO effect that doubles the frequency. 2D-ALBF keeps the infinite planar [Be2BO3F2](infinity) structure in KBBF but does not contain the toxic beryllium element.