Access to the elusive deep-ultraviolet by direct second harmonic generation (SHG) enabled by a new beryllium-free zincoborate-phosphate crystal is reported. Ba-3(ZnB5O10)PO4, exhibits large SHG responses at 1064 and 532 nm and a short 180 nm absorption edge. Centimeter-size crystals are grown, and quantum mechanical calculations demonstrate the key role played by ZnO4 tetrahedra in the enhanced optical responses.