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Planar MO 3 (M = B, C, N) units have frequently been considered important structural components of novel birefringent crystal materials. An efficient approach for constructing new functional crystals is to simultaneously assemble multiple structural motifs together. Two compounds, Na 3 Rb 6 (CO 3 ) 3 (NO 3 ) 2 X·6H 2 O (X = Br and Cl), were synthesized by the integration of three kinds of anionic groups. More interestingly, the [CO 3 ] 2− and [NO 3 ] − groups in Na 3 Rb 6 (CO 3 ) 3 (NO 3 ) 2 X·6H 2 O are all coplanar with the aid of [NaO 7 ] 13− polyhedra, which can enhance the anisotropic polarizability. Na 3 Rb 6 (CO 3 ) 3 (NO 3 ) 2 X·6H 2 O have a large theoretical birefringence of ∼0.165 at 1064 nm and possess a short UV cut-off edge of ∼230 nm. Additionally, the two compounds exhibit good crystal growth habits. These properties illustrate that Na 3 Rb 6 (CO 3 ) 3 (NO 3 ) 2 X·6H 2 O are promising UV birefringent crystals.