The 0.74Na1/2Bi1/2TiO3‐0.26SrTiO3 co‐doped with Li2CO3 and B2O3 are studied to develop the low‐temperature sintered lead‐free piezoceramic for multilayer applications. The studied piezoceramics are synthesized by a conventional solid‐state reaction method. Their crystal structures, microstructures, ferroelectrics, and strain properties are analyzed. Interestingly. the addition of Li2CO3 and B2O3 reduces the sintering temperature of the 0.74Na1/2Bi1/2TiO3‐0.26SrTiO3 sample from 1175oC to 975oC. All samples show a pseudo‐cubic perovskite structure with a dense microstructure and an inhomogeneous grain size distribution. The electric‐field‐induced polarization loops of the samples are saturated at 4 kV/mm. More importantly, the 0.74Na1/2Bi1/2TiO3‐0.26SrTiO3 + 1wt%Li2CO3 + 1wt%B2O3 sample sintered at 975oC shows a Smax/Emax value of 510 pm/V under an applied electric field of 2 kV/mm, which is promising for multilayer lead‐free piezoelectric actuator applications.This article is protected by copyright. All rights reserved.