Abstract Perovskite oxides are promising thermal barrier coatings (TBCs) materials but their thermophysical properties still need to be further improved before commercial applications. In this work, mechanical/thermal properties of calcium‐strontium zirconate solid solutions (Ca 1− x Sr x ZrO 3 ) are investigated. Comparing to the end‐compounds CaZrO 3 and SrZrO 3 , the solid solutions achieve the enhanced thermal expansion coefficient, decreased thermal conductivity as well as good high‐temperature mechanical properties. The experimental thermal conductivities of Ca 1− x Sr x ZrO 3 ( x = 0.2, 0.4, 0.6, 0.8) are in the range of 1.76‐1.94 W·(m·K) −1 at 1073 K, being lower than that of the yttria‐stabilized zirconia (YSZ). At the same time, their thermal expansion coefficients (10.75 × 10 −6 ‐11.23 × 10 −6 /K at 1473 K) are comparable to that of YSZ. Moreover, the Young's moduli of Ca 0.8 Sr 0.2 ZrO 3 , Ca 0.6 Sr 0.4 ZrO 3 , Ca 0.4 Sr 0.6 ZrO 3 , and Ca 0.2 Sr 0.8 ZrO 3 at 1473 K are 70.7%, 69.4%, 68.8%, and 71.1% of the corresponding values at room temperature, respectively. The good high‐temperature mechanical and thermal properties ensure the potential applications of Ca 1− x Sr x ZrO 3 solid solutions as high‐temperature thermal insulation materials including TBCs.