Combining simultaneous substitution of Ca and Sr for the La site in LaCrO3 and pulverization of calcined particles with planet-type yttria-stabilized ZrO2 ball mill La0.70Ca0.30-xSrxCrO3, ceramics with sintering density of more than 93% were successfully prepared. Not only sintering properties but also structural phase transition behavior, such as temperature, variation of enthalpy, and entropy, of La1-x-yCaxSryCrO3 could be controlled by alkaline earth composition. The variation of the transition behavior on Sr content could be fairly explained with the model, assuming that the phase with high crystal symmetry has high thermodynamic stability, i.e., low standard Gibbs energy of formation. Because La0.70Ca0.05Sr0.25CrO3 not only has high sintering properties but also no structural phase transition between room temperature to solid oxide fuel cell (SOFC) operation and equal electrical conductivity to that of La0.70Ca0.35CrO3, which was reported to be a promising material for SOFC interconnectors, it can be expected that La0.70Ca0.05Sr0.25CrO3 is a superior candidate to La0.70Ca0.35CrO3 as interconnector material for SOFCs. (c) 2008 The Electrochemical Society.