New temperature stability Ba1−xSrxV2O6 (0.35 ≤ x ≤ 0.55) microwave dielectric ceramics prepared by the conventional solid-state route were investigated. X-ray diffraction confirmed that all the specimens formed a solid solution single phase with orthorhombic structure. The microwave dielectric properties strongly depended on the compositions, densification and microstructure of the specimens. Furthermore, partial Sr ions substitution for Ba ions in Ba1−xSrxV2O6 lattices not only successfully improved the temperature stability of BaV2O6-based ceramic but also promoted the sinterability of SrV2O6-based one. Out of these compositions, Ba0.5Sr0.5V2O6 sintered at 625 °C exhibited a near-zero τf together with a low permittivity εr ~ 11.5 and a quality factor Q × f ~ 14 100 GHz, which also showed good chemical compatibility with Al electrodes.