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Sintering for large‐sized, stoichiometric Bi0.5Na0.5TiO3 (BNT) ceramics is of great challenge due to the loss of volatile Bi/Na at A‐site of perovskite structure. In this work, BNT ceramic tile with the size of ∼10 × 10 cm2 and near‐stoichiometric composition has been successfully fabricated by Isobam‐assisted gelcasting process, followed by sintering with 1150°C calcined power bed. The powder bed...