Nonlinear optical (NLO) materials are of great importance in laser science and technology, as they can expand the wavelength range provided by common laser sources. Few NLO materials, except KBe2BO3F2 (KBBF), can practically generate deep-ultraviolet coherent light by direct second-harmonic generation process, limited by the fundamental requirements on the structure-directing optical properties. However, KBBF suffers a strong layering tendency and high toxicity of the containing beryllium, which hinder the commercial availability of KBBF. Here we report a new beryllium-free borate, Li4Sr(BO3)2, which preserves the structural merits of KBBF, resulting in the desirable optical properties. Furthermore, Li4Sr(BO3)2 mitigates the layering tendency greatly and enhances the efficiency of second-harmonic generation by more than half that of KBBF. These results suggest that Li4Sr(BO3)2 is an attractive candidate for the next generation of deep-ultraviolet NLO materials. This beryllium-free borate represents a new research direction in the development of deep-ultraviolet NLO materials.