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In this work, two perovskite‐type compounds, K0.5Bi0.5TiO3 and LaAlO3, have been selected as host material to incorporate with BiAlO3 using a solid‐state reaction route. The phase evolution and dielectric properties for both systems have been investigated in detail. For the K0.5Bi0.5TiO3BiAlO3 system, it is interesting to find that when using Bi2O3, Al2O3, K2CO3, and TiO2 as starting materials, the...