The first mixed alkali metal borosulfate compound, Li2NaB3S2O12 (LNBSO), which contains [BO3] groups, was designed and synthesized by using a high boron-to-sulfur ratio strategy through the high temperature solution method. LNBSO exhibits a birefringence of 0.057@546.1 nm in experiments, which was mainly contributed by the [BO3] groups, and possesses a short absorption edge at 184 nm, and the space group of LNBSO is P21/c. This newly synthesized borosulfate compound holds potential as a promising birefringent material within the deep-ultraviolet wavelength range. Moreover, the investigation on the relationship among the ratio of boron to sulfur, the dimensionality of the anionic framework, and the formation of [BO3] groups has been conducted on available borosulfate, providing insights for the synthesis of borosulfate with desirable performances.