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.　©　2024　Science　China　Press