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The prototypical Ruddlesden‐Popper compound Ca3Mn2O7 has been predicted to possess hybrid improper ferroelectricity, where the polarization is induced by the condensation of two oxygen octahedral distortion modes. Nevertheless, it is a big challenge to switch the polarization at room temperature in Ca3Mn2O7 since the presence of intermediate nonpolar Acaa phase generally leads to the complex domain...