There　is　a　pressing　demand　for　the　development　of　novel　birefringent　crystals　tailored　for　compact　optical　components,　especially　for　crystals　exhibiting　large　birefringence　across　a　range　of　temperatures.　This　has　commonly　been　achieved　by　introducing　various　deformable　groups　with　high　polarizability　anisotropy.　In　this　study,　we　combined　both　rigid　and　deformable　groups　to　synthesise　a　new　birefringent　crystal,　Al2Te2MoO10,　which　demonstrates　an　exceptional　birefringence　value　of　0.29@550　nm　at　room　temperature.　Not　only　is　this　higher　birefringence　than　that　of　commercial　crystals,　but　Al2Te2MoO10　exhibits　excellent　birefringence　stability　over　a　wide　temperature　range,　from　123　to　503　K.　In　addition,　the　first-principles　theory　calculations　and　structural　analyses　suggest　that　although　the　rigid　AlO6　groups　do　not　make　much　contribution　to　the　prominent　birefringence,　they　nonetheless　played　a　role　in　maintaining　the　structural　anisotropy　at　elevated　temperatures.　Based　on　these　findings,　this　paper　proposes　a　novel　structural　design　strategy　to　complement　conventional　approaches　for　developing　optimal　birefringent　crystals　under　various　environmental　conditions.　(c)　2024　Science　China　Press.　Published　by　Elsevier　B.V.　and　Science　China　Press.　All　rights　are　reserved,　including　those　for　text　and　data　mining,　AI　training,　and　similar　technologies.