In recent years, birefringent crystals have attracted much attention in the field of optical materials and play a significant role in laser technology and optical imaging. However, commercially available birefringent crystals are still relatively scarce and need improvement. Low-dimensional structures and well-oriented anisotropic units are conducive to obtaining excellent birefringent materials. Therefore, it is crucial to utilize a molecular engineering strategy for designing crystal structures. Through screening, the tellurite-nitrate system caught our attention because most of them exhibit low dimensional structures. The structure of Hg